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2019-07-31
The Effect of Chemical Disorder on Defect Formation and Migration in Disordered MAX Phases
MAX phases have attracted increased attention due to their unique combination of ceramic and metallic properties. Point-defects are known to play a vital role in the structural, electronic and transport properties of alloys in general and this system in particular. As some MAX phases have been shown to be stable in non-stoichiometric compositions, it is likely that such alloying effects will affect the behavior of lattice point defects. This problem, however, remains relatively unexplored. In this work, we investigate the alloying effect on the structural-stability, energy-stability, electronic-structure, and diffusion barrier of point defects in MAX phase alloys within a first-principles density functional theory framework. The vacancy (V$_{M}$, V$_{A}$, V$_{X}$) and antisite (M-A; M-X) defects are considered with M and A site disorder in (Zr-M)$_{2}$(AA${'}$)C, where M=Cr,Nb,Ti and AA${'}$=Al, Al-Sn, Pb-Bi. Our calculations suggest that the chemical disorder helps lower the V$_{A}$ formation energies compared to V$_{M}$ and V$_{X}$. The V$_{A}$ diffusion barrier is also significantly reduced for M-site disorder compared to their ordered counterpart. This is very important finding because reduced barrier height will ease the Al diffusion at high-operating temperatures, which will help the formation of passivating oxide layer (i.e., Al$_{2}$O$_{3}$ in aluminum-based MAX phases) and will slow down or stop the material degradation. We believe that our study will provide a fundamental understanding and an approach to tailor the key properties that can lead to the discovery of new MAX phases.
1908.00038v3
2019-08-02
Tunable Electronic Structure in Gallium Chalcogenide van der Waals Compounds
Transition metal monochalcogenides comprise a class of two-dimensional materials with electronic band gaps that are highly sensitive to material thickness and chemical composition. Here, we explore the tunability of the electronic excitation spectrum in GaSe using angle-resolved photoemission spectroscopy. The electronic structure of the material is modified by $\textit{in-situ}$ potassium deposition as well as by forming GaS$_{x}$Se$_{1-x}$ alloy compounds. We find that potassium decouples the top-most tetra-layer of the GaSe unit cell, leading to a substantial change of the dispersion around the valence band maximum (VBM). The observed band dispersion of a single tetralayer is consistent with a transition from the direct gap character of the bulk to the indirect gap character expected for monolayer GaSe. Upon alloying with sulfur, we observe a phase transition from AB to $\text{AA}^{\prime}$ stacking. Alloying also results in a rigid energy shift of the VBM towards higher binding energies which correlates with a blue shift in the luminescence. The increase of the band gap upon sulfur alloying does not appear to change the dispersion or character of the VBM appreciably, implying that it is possible to engineer the gap of these materials while maintaining their salient electronic properties.
1908.01003v2
2019-08-05
Prediction of a wide variety of linear complexions in face centered cubic alloys
Linear complexions are defect states that have been recently discovered along dislocations in body centered cubic Fe-based alloys. In this work, we use atomistic simulations to extend this concept and explore segregation-driven structural transitions at dislocations in face centered cubic alloys. We identify a variety of stable, nanoscale-size structural and chemical states, which are confined near dislocations and can be classified as linear complexions. Depending on the alloy system and thermodynamic conditions, such new states can preserve, partially modify, or completely replace the original defects they were born at. By considering different temperatures and compositions, we construct linear complexion diagrams that are similar to bulk phase diagrams, defining the important conditions for complexion formation while also specifying an expected complexion size and type. Several notable new complexion types were predicted here: (1) nanoparticle arrays comprised of L12 phases in Ni-Fe, Ni-Al, and Al-Zr, (2) replacement of stacking faults with layered complexions comprised of (111) planes from the Cu5Zr intermetallic phase in Cu-Zr, (3) platelet arrays comprised of two-dimensional Guinier-Preston zones in Al-Cu, and finally (4) coexistence of multiple linear complexions containing both Guinier-Preston zones and L12 phases in ternary Al-Cu-Zr. All of these new complexion states are expected to alter material properties and affect the stability of the dislocations themselves, offering a unique opportunity for future materials design.
1908.01849v2
2019-09-07
Lithiation-delithiation cycles of amorphous Si nanowires investigated by molecular dynamics simulations
The atomistic mechanisms during lithiation and delithiation of amorphous Si nanowires ($a$-SiNW) have been investigated over cycles by molecular dynamics simulations. First, the Modified Embedded Atom Method (MEAM) potential from Cui et al. [J. Power Sources. 2012, (207) 150] has been further optimized on static (Li$_x$Si alloy phases and point defect energies) and on dynamic properties (Li diffusion) to reproduce the lithiation of small crystalline Si nanowires calculated at the {\it ab initio} level. The lithiation of $a$-SiNW reveals a two-phase process of lithiation with a larger diffusion interface compared to crystalline Si lithiation. Compressive axial stresses are observed in the amorphous Si$_x$Li alloy outer shell. They are easily released thanks to the soft glassy behavior of the amorphous alloy. Conversely, in crystalline SiNW, the larger stress in the narrow crystalline lithiated interface is hardly released and requires a phase transformation to amorphous to operate, which delays the lithiation. The history of the charge-discharge cycles as well as the temperature appear as driving forces for phase transformation from amorphous Li$_x$Si alloy to the more stable crystalline phase counterpart. Our work suggest that a full delithiation could heal the SiNWs to improve the life cycles of Li-ion batteries with Si anode.
1909.03268v1
2019-12-07
Effect of chemical disorder on the electronic stopping of solid solution alloys
The electronic stopping power of nickel-based equiatomic solid solutions alloys NiCr, NiFe and NiCo for protons and alpha projectiles is investigated in detail using real-time time-dependent density functional theory over a wide range of velocities. Recently developed numerical electronic structure methods are used to probe fundamental aspects of electron-ion coupling non-perturbatively and in a fully atomistic context, capturing the effect of the atomic scale disorder. The effects of particular electronic band structures and density of states reflect in the low velocity limit behavior. We compare our results for the alloys with those of a pure nickel target to understand how alloying affects the electronic stopping. We discover that NiCo and NiFe have similar stopping behavior as Ni while NiCr has an asymptotic stopping power that is more than a factor of two larger than its counterparts for velocities below 0.1 a.u.. We show that the low-velocity limit of electronic stopping power can be manipulated by controlling the broadening of the d-band through the chemical disorder. In this regime, the Bragg's additive rule for the stopping of composite materials also fails for NiCr.
1912.03399v2
2019-12-18
Fast and stable deep-learning predictions of material properties for solid solution alloys
We present a novel deep learning (DL) approach to produce highly accurate predictions of macroscopic physical properties of solid solution binary alloys and magnetic systems. The major idea is to make use of the correlations between different physical properties in alloy systems to improve the prediction accuracy of neural network (NN) models. We use multitasking NN models to simultaneously predict the total energy, charge density and magnetic moment. These physical properties mutually serve as constraints during the training of the multitasking NN, resulting in more reliable DL models because multiple physics properties are correctly learned by a single model. Two binary alloys, copper-gold (CuAu) and iron-platinum (FePt), were studied. Our results show that once the multitasking NN's are trained, they can estimate the material properties for a specific configuration hundreds of times faster than first-principles density functional theory calculations while retaining comparable accuracy. We used a simple measure based on the root-mean-squared errors (RMSE) to quantify the quality of the NN models, and found that the inclusion of charge density and magnetic moment as physical constraints leads to more stable models that exhibit improved accuracy and reduced uncertainty for the energy predictions.
1912.11152v3
2019-12-24
Influence of thermomechanical loads on the energetics of precipitation in magnesium aluminum alloys
We use first principles calculations to study the influence of thermomechanical loads on the energetics of precipitation in magnesium-aluminum alloys. Using Density Functional Theory simulations, we present expressions of the energy of magnesium-aluminum binary solid solutions as a function of concentration, strain and temperature. Additionally, from these calculations, we observe an increase in equilibrium volume (and hence the equilibrium lattice constants) with the increase in concentration of magnesium. We also observe an increase in the cohesive energy of solutions with increase in concentration, and also present their dependence on strain. Calculations also show that the formation enthalpy of $\beta$ phase solutions to be strongly influenced by hydrostatic stress, however the formation enthalpy of $\alpha$ phase solutions remain unaffected by hydrostatic stress. We present an expression of the free energy of any magnesium aluminum solid solution, that takes into account the contributions of strain and temperature. We note that these expressions can serve as input to process models of magnesium-aluminum alloys. We use these expressions to report the influence of strains and temperature on the solubility limits and equilibrium chemical potential in Mg-Al alloys. Finally, we report the influence of thermomechanical loads on the growth of precipitates, where we observe compressive strains along the $c$ axis promotes growth, whereas strains along the $a$ and $b$ directions do not influence the growth of precipitates.
1912.11434v2
2020-02-17
Ductile and brittle crack-tip response in equimolar refractory high-entropy alloys
Understanding the strengthening and deformation mechanisms in refractory high-entropy alloys (HEAs), proposed as new high-temperature material, is required for improving their typically insufficient room-temperature ductility. Here, density-functional theory simulations and a continuum mechanics analysis were conducted to systematically investigate the competition between cleavage decohesion and dislocation emission from a crack tip in the body-centered cubic refractory HEAs HfNbTiZr, MoNbTaVW, MoNbTaW, MoNbTiV, and NbTiVZr. This crack-tip competition is evaluated for tensile loading and a totality of 15 crack configurations and slip systems. Our results predict that dislocation plasticity at the crack tip is generally unfavorable -- although the competition is close for some crack orientations, suggesting intrinsic brittleness and low crack-tip fracture toughness in these five HEAs at zero temperature. Fluctuations in local alloy composition, investigated for HfNbTiZr, can locally reduce the resistance to dislocation emission for a slip system relative to the configuration average of that slip system, but do not change the dominant crack-tip response. In the case of single-crystal MoNbTaW, where an experimental, room-temperature fracture-toughness value is available for a crack on a \{100\} plane, theoretical and experimental results agree favorably. Factors that may limit the agreement are discussed. We survey the effect of material anisotropy on preferred crack tip orientations, which are found to be alloy specific. Mixed-mode loadings are found to shift the competition in favor of cleavage or dislocation nucleation, depending on crack configuration and amplified by the effect of material anisotropy on crack tip stresses.
2002.07013v1
2020-06-09
Orbital-enhanced Warping Effect in P\textsubscript{x},P\textsubscript{y}-derived Rashba Spin Splitting of Monatomic Bismuth Surface Alloy Surface Alloy
Spin-split Rashba bands have been exploited to efficiently control the spin degree of freedom of moving electrons, which possesses a great potential in frontier applications of designing spintronic devices and processing spin-based information. Given that intrinsic breaking of inversion symmetry and sizeable spin-orbit interaction, two-dimensional (2D) surface alloys formed by heavy metal elements exhibit a pronounced Rashba-type spin splitting of the surface states. Here, we have revealed the essential role of atomic orbital symmetry in the hexagonally warped Rashba spin-split surface state of $\sqrt{3}\times\sqrt{3} R30^{\circ}$ BiCu$_{2}$ monatomic alloy by scanning tunneling spectroscopy (STS) and density functional theory (DFT). From $\mathrm{d}I/\mathrm{d}U$ spectra and calculated band structures, three hole-like Rashba-split bands hybridized from distinct orbital symmetries have been identified in the unoccupied energy region. Because of the hexagonally deformed Fermi surface, quasi-particle interference (QPI) mappings have resolved scattering channels opened from interband transitions of \textit{p$_{x},$p$_{y}$}($m_{j}=1/2$) band. In contrast to the \textit{s,p$_{z}$}-derived band, the hexagonal warping predominately is accompanied by substantial out-of-plane spin polarization $S_{z}$ up to 24\% in the dispersion of \textit{p$_{x}$,p$_{y}$}($m_{j}=1/2$) band with an in-plane orbital symmetry.
2006.05024v1
2020-07-30
Elastic dipole tensors and relaxation volumes of point defects in concentrated random magnetic Fe-Cr alloys
Point defects in body-centred cubic Fe, Cr and concentrated random magnetic Fe-Cr are investigated using density functional theory and theory of elasticity. The volume of a substitutional Cr atom in ferromagnetic bcc Fe is approximately 18\% larger than the volume of a host Fe atom, whereas the volume of a substitutional Fe atom in antiferromagnetic bcc Cr is 5\% smaller than the volume of a host Cr atom. Elastic dipole $\boldsymbol{P}$ and relaxation volume $\boldsymbol{\Omega}$ tensors of vacancies and self-interstitial atom (SIA) defects exhibit large fluctuations, with vacancies having negative and SIA large positive relaxation volumes. Dipole tensors of vacancies are nearly isotropic across the entire alloy composition range, with diagonal elements $P_{ii}$ decreasing as a function of Cr content. Fe-Fe and Fe-Cr SIA dumbbells are more anisotropic than Cr-Cr dumbbells. Fluctuations of elastic dipole tensors of SIA defects are primarily associated with the variable crystallographic orientations of the dumbbells. Statistical properties of tensors $\boldsymbol{P}$ and $\boldsymbol{\Omega}$ are analysed using their principal invariants, suggesting that point defects differ significantly in alloys containing below and above 10\% at. Cr. The relaxation volume of a vacancy depends sensitively on whether it occupies a Fe or a Cr lattice site. A correlation between elastic relaxation volumes and magnetic moments of defects found in this study suggests that magnetism is a significant factor influencing elastic fields of defects in Fe-Cr alloys.
2007.15424v1
2020-09-17
Hydride growth mechanism in Zircaloy-4: investigation of the partitioning of alloying elements
The long-term safety of water-based nuclear reactors relies in part on the reliability of zirconium-based nuclear fuel. Yet the progressive ingress of hydrogen during service makes zirconium alloys subject to delayed hydride cracking. Here, we use a combination of electron back-scattered diffraction and atom probe tomography to investigate specific microstructural features from the as-received sample and in the blocky-alpha microstructure, before and after electrochemical charging with hydrogen or deuterium followed by a low temperature heat treatment at 400C for 5 hours followed by furnace cooling at a rate of 0. 5C per min. Specimens for atom probe were prepared at cryogenic temperature to avoid the formation of spurious hydrides. We report on the compositional evolution of grains and grain boundaries over the course of the sample's thermal history, as well as the ways the growth of the hydrides modifies locally the composition and the structure of the alloy. We observe a significant amount of deuterium left in the matrix, even after the slow cooling and growth of the hydrides. Stacking faults form ahead of the growth front and Sn segregates at the hydride-matrix interface and on these faults. We propose that this segregation may facilitate further growth of the hydride. Our systematic investigation enables us discuss how the solute distribution affects the evolution of the alloy's properties during its service lifetime.
2009.08073v1
2020-09-27
Exploring In$_2$(Se$_{1-x}$Te$_x$)$_3$ alloys as photovoltaic materials
In$_2$Se$_3$ in the three-dimensional (3D) hexagonal crystal structure with space group $P6_1$ ($\gamma$-In$_2$Se$_3$) has a direct band gap of $\sim$1.8 eV and high absorption coefficient, making it a promising semiconductor material for optoelectronics. Incorporating Te allows for tuning the band gap, adding flexibility to device design and extending the application range. Here we report the growth and characterization of $\gamma$-In$_2$Se$_3$ thin films, and results of hybrid density functional theory calculations to assess the electronic and optical properties of $\gamma$-In$_2$Se$_3$ and $\gamma$-In$_2$(Se$_{1-x}$Te$_x$)$_3$ alloys. The calculated band gap of 1.84 eV for $\gamma$-In$_2$Se$_3$ is in good agreement with data from the absorption spectrum, and the absorption coefficient is found to be as high as that of direct band gap conventional III-V and II-VI semiconductors. Incorporation of Te in the form of $\gamma$-In$_2$(Se$_{1-x}$Te$_x$)$_3$ alloys is an effective way to tune the band gap from 1.84 eV down to 1.23 eV, thus covering the optimal band gap range for solar cells. We also discuss band gap bowing and mixing enthalpies, aiming at adding $\gamma$-In$_2$Se$_3$ and $\gamma$-In$_2$(Se$_{1-x}$Te$_x$)$_3$ alloys to the available toolbox of materials for solar cells and other optoelectronic devices.
2009.12885v2
2020-10-22
Computational property predictions of Ta-Nb-Hf-Zr high-entropy alloys
Refractory high entropy alloys (R-HEAs) are having properties and uses as high strength and high hardness materials for ambient and high temperature, aerospace and nuclear radiation tolerance applications, orthopedic applications etc. The mechanical properties like yield strength and ductility of TaNbHfZr R-HEA depend on the local nanostructure and chemical ordering. In this study we have computationally obtained various properties of the TaNbHfZr alloy like the role of configurational entropy in the thermodynamic property, rate of evolution of nanostructure morphology in thermally annealed systems, dislocation simulation based quantitative prediction of yield strength, nature of dislocation movement through short range clustering (SRC) and qualitative prediction of ductile to brittle transition behavior. The simulation starts with hybrid Monte Carlo/ Molecular Dynamics (MC/MD) based nanostructure evolution of an initial random solid solution alloy structure with BCC lattice structure created with principal axes along [1 1 1], [-1 1 0] and [-1 -1 2] directions suitable for simulation of 1/2[1 1 1] edge dislocations. Thermodynamic properties are calculated from the change in enthalpy and the configurational entropy by next-neighbor bond counting statistics. The MC/MD evolved structures mimic the annealing treatment at 1800{\deg}C and the output structures are replicated in periodic directions to make larger 384000 atom structures used for dislocation simulations. Edge dislocations were utilized to obtain and explain for the extra strengthening observed because of the formations of SRCs. Lastly the MC/MD evolved structures containing dislocations are subjected to a high shear stress beyond CRSS to investigate the stability of the dislocations and the lattice structures to explain the experimentally observed transition from ductile to brittle behavior for the TaNbHfZr R-HEA.
2010.11772v1
2020-12-03
Effect of ageing on the properties of the W-containing IRIS-TiAl alloy
The effects of ageing at 800 $^\circ$C on the properties of the IRIS alloy (Ti$_{49.9}$Al$_{48}$W$_2$B$_{0.1}$) are studied. The initial microstructure of this alloy densified by Spark Plasma Sintering (SPS) is mainly composed of lamellar colonies which are surrounded by $\gamma$ grains. The evolutions of the alloy strength and creep resistance resulting from this ageing treatment are measured by the related mechanical tests. The microstructural changes are investigated by scanning and transmission electron microscopies and by X-ray diffraction. The main structural evolutions consist in a shrinkage of the lamellar areas and in a precipitation of $\beta_0$ phase, which is accompanied by a moderate segregation of tungsten and a decrease of the $\alpha_2$ lamellar width. However, these evolutions are relatively limited and the microstructural stability is found to result mainly from the low diffusivity of tungsten. Conversely, a moderate effect of this ageing treatment on mechanical properties, at room and high temperatures, is measured. Such experimental results are interpreted and discussed in terms of the microstructural evolutions and of the deformation mechanisms which are activated at different temperatures under various solicitations.
2012.01760v1
2020-12-18
Aging behavior of Haynes 282 wrought nickel superalloy subjected to a cold pre-deformation by differential speed rolling
The mechanical response of Haynes 282, a wrought gamma prime strengthened nickel based superalloy, is tailored by using both a cold deformation processing and a post straining heat treatment including a two step aging. In this work, the effect of the applied cold pre deformation by conventional equal speed rolling ESR or differential speed rolling DSR methods on the aging behavior of Haynes 282 superalloy, is examined for the first time. For this reason, the solid solution annealed alloy was subjected to 50 pct. nominal cold thickness reduction by either ESR or DSR methods, followed by a two step heat treatment at 1010C for 2h and 780C for 8h. The material structural evolution on each processing step was characterized by using scanning electron microscopy, electron backscatter diffraction and transmission electron microscopy methods. Corresponding mechanical properties were examined in static tensile tests performed on non standard miniaturized specimens. It was found that, the introduction of a shear strain by rolls speed differentiation in the cold rolling process results in a more efficient strain hardening of the alloy in the as deformed state and an intensive grain refinement upon the post deformation annealing. Consequently, the DSR provides a higher room temperature mechanical strength obtained in both aging steps, as compared to the non deformed and conventionally cold rolled counterparts. Furthermore, noticeable differences in terms of stability of crystallographic orientations for ESRed or DSRed and heat treated alloy, were noted.
2012.10114v1
2021-01-12
Reactivity of transition-metal alloys to oxygen and sulphur
Oxidation and tarnishing are the two most common initial steps in the corrosive process of metals at ambient conditions. These are always initiated with O and S binding to a metallic surface, so that one can use the binding energy as a rough proxy for the metal reactivity. With this in mind, we present a systematic study of the binding energy of O and S across the entire transition-metals composition space, namely we explore the binding energy of {\bf 88} single-phase transition metals and of {\bf 646} transition-metal binary alloys. The analysis is performed by defining a suitable descriptor for the binding energy. This is here obtained by fitting several schemes, based on the original Newns-Anderson model, against density-functional-theory data for the 4$d$ transition metal series. Such descriptor is then applied to a vast database of electronic structures of transition-metal alloys, for which we are able to predict the range of binding energies across both the compositional and the structural space. Finally, we extend our analysis to ternary transition-metal alloys and identify the most resilient compounds to O and S binding.
2101.04767v2
2021-05-01
Density functional simulations of pressurized Mg-Zn and Al-Zn alloys
The Mg-Zn and Al-Zn binary alloys have been investigated theoretically under static isotropic pressure. The stable phases of these binaries on both initially hexagonal-close-packed (HCP) and face-centered-cubic (FCC) lattices have been determined by utilizing an iterative approach that uses a configurational cluster expansion method, Monte Carlo search algorithm, and density functional theory (DFT) calculations. Based on 64-atom models, it is shown that the most stable phases of the Mg-Zn binary alloy under ambient condition are $\rm MgZn_3$, $\rm Mg_{19}Zn_{45}$, $\rm MgZn$, and $\rm Mg_{34}Zn_{30}$ for the HCP, and $\rm MgZn_3$ and $\rm MgZn$ for the FCC lattice, whereas the Al-Zn binary is energetically unfavorable throughout the entire composition range for both the HCP and FCC lattices under all conditions. By applying an isotropic pressure in the HCP lattice, $\rm Mg_{19}Zn_{45}$ turns into an unstable phase at P$\approx$$10$~GPa, a new stable phase $\rm Mg_{3}Zn$ appears at P$\gtrsim$$20$~GPa, and $\rm Mg_{34}Zn_{30}$ becomes unstable for P$\gtrsim$$30$~GPa. For FCC lattice, the $\rm Mg_{3}Zn$ phase weakly touches the convex hull at P$\gtrsim$$20$~GPa while the other stable phases remain intact up to $\approx$$120$~GPa. Furthermore, making use of the obtained DFT results, bulk modulus has been computed for several compositions up to pressure values of the order of $\approx$$120$~GPa. The findings suggest that one can switch between $\rm Mg$-rich and $\rm Zn$-rich early-stage clusters simply by applying external pressure. $\rm Zn$-rich alloys and precipitates are more favorable in terms of stiffness and stability against external deformation.
2105.00209v1
2021-05-10
A Novel Smart Memory Alloy Re-centering Damper for Passive Protection of Structures Subjected to Seismic Excitations Using High-Performance NiTiHfPd Material
This research proposes and evaluates a superelastic memory alloy re-centering damper system for improving the reaction of steel frame buildings that have been exposed to several levels of seismic threat. The planned superelastic memory alloy re-centering damper (SMARD) relies on high-performance shape memory alloy (SMA) bars for its abilities of recentering and augments its deformation potential with friction springs. To begin, this study investigates the superelastic reaction of NiTiHfPd SMAs under a variety of conditions and shows how they can be used in seismic applications. To gather experimental results, uniaxial experiments on superelastic NiTiHfPd SMAs are performed at temperatures ranging from -35 to 25 oC and loading frequencies ranging from 0.05 to 1 Hz with four distinct strain amplitudes. We explore the impact of loading rate and temperature on the superelastic properties of NiTiHfPd SMAs. The complex answer of 6-floor and 9-floor steel special moment frame buildings with built SMARDs is then determined using an empirical model. Finally, nonlinear reaction time background simulations are used to characterize the actions of managed and unregulated buildings while 44 ground motion data are used. The results indicate that SMARDs will significantly reduce the dynamic behavior of steel-frame buildings at various seismic threat levels while simultaneously improving their post-earthquake functionality.
2105.04081v1
2021-05-10
The high temperature mechanical properties and the correlated microstructure/texture evolutions of a TWIP high entropy alloy
The present work deals with the microstructure and texture evolutions of a TWIP high entropy alloy at various temperatures. Toward this end, the tensile tests were conducted at temperatures ranging from 298 to 873 K under the strain rate of 0.001s-1. The experimented material exhibited an extraordinary room temperature work hardening behavior, in respect of both the instantaneous strain hardening exponent and the work hardening rate values. This resulted in an acceptable ultimate tensile strength /ductility balance and was justified considering the high activity of twinning and planar slip. Such work hardening capacity deteriorated at higher temperatures due to increasing the dislocation annihilation rate and the stacking fault energy values that suppressed twin formation and dislocation accumulation. However, the decrease in amplitude and extent of the work hardening region was insignificant compared with other single-phase high entropy alloys. This was attributed to the high capacity of the alloy for dislocation storage at various deformation temperatures. The serrated flow was observed at 773 and 873 K due to the dynamic strain aging (DSA) mechanism. Interestingly, in this case, the DSA mechanism has a beneficial effect on overall ductility, which was attributed to the increase in the strain hardening exponent result in a delay of necking. Texture examination also reveals the formation of a double fiber texture due to the simultaneous contribution of twinning and octahedral slip.
2105.04597v1
2021-05-17
Thermo-magnetic characterization of phase transitions in a Ni-Mn-In metamagnetic shape memory alloy
The partially overlapped ferroelastic/martensitic and para-ferromagnetic phase transitions of a Ni$_{50.53}$Mn${33.65}$In$_{15.82}$ metamagnetic shape memory alloy have been studied from calorimetric, magnetic and acoustic emission measurement. We have taken advantage of the existence of thermal hysteresis of the first order ferroelastic/martensitic phase transition ($\sim2.5$K) to discriminate the latent heat contribution $\Delta$Ht = 7.21(15) kJ/kg and the specific heat contribution $\Delta$Hc = 216(1) J/kg to the total excess enthalpy of the phase transition. The specific heat was found to follow a step-like behavior at this phase transition. The intermittent dynamics of the ferroelastic/martensitic transition has been characterized as a series of avalanches detected both from acoustic emission and calorimetric measurements. The energy distribution of these avalanche events was found to follow a power law with a characteristic energy exponent $\epsilon\sim2$ which is in agreement with the expected value for a system undergoing a symmetry change from cubic to monoclinic. Finally, the critical behavior of the para-ferromagnetic austenite phase transition that takes place at $\sim 311$K has been studied from the behavior of the specific heat. A critical exponent $\alpha\sim0.09$ has been obtained, which has been shown to be in agreement with previous values reported for Ni-Mn-Ga alloys but different from the critical divergence reported for pure Ni.
2105.07916v2
2021-05-31
Tunable Two-Dimensional Group-III Metal Alloys
Chemically stable quantum-confined 2D metals are of interest in next-generation nanoscale quantum devices. Bottom-up design and synthesis of such metals could enable the creation of materials with tailored, on-demand, electronic and optical properties for applications that utilize tunable plasmonic coupling, optical non-linearity, epsilon-near-zero behavior, or wavelength-specific light trapping. In this work, we demonstrate that the electronic, superconducting and optical properties of air-stable two-dimensional metals can be controllably tuned by the formation of alloys. Environmentally robust large-area two-dimensional InxGa1-x alloys are synthesized by Confinement Heteroepitaxy (CHet). Near-complete solid solubility is achieved with no evidence of phase segregation, and the composition is tunable over the full range of x by changing the relative elemental composition of the precursor. The optical and electronic properties directly correlate with alloy composition, wherein the dielectric function, band structure, superconductivity, and charge transfer from the metal to graphene are all controlled by the indium/gallium ratio in the 2D metal layer.
2106.00117v1
2021-06-18
Design Principles for High Temperature Superconductors with Hydrogen-based Alloy Backbone at Moderate Pressure
Hydrogen-based superconductors provide a route to the long-sought goal of room-temperature superconductivity, but the high pressures required to metallize these materials limit their immediate application. For example, carbonaceous sulfur hydride, the first room-temperature superconductor, can reach a critical temperature (Tc) of 288 K only at the extreme pressure of 267 GPa. The next recognized challenge is the realization of room-temperature superconductivity at significantly lower pressures. Here, we propose a strategy for the rational design of high-temperature superconductors at low pressures by alloying small-radius elements and hydrogen to form ternary hydride superconductors with alloy backbones. We identify a hitherto unknown fluorite-type backbone in compositions of the form AXH8, which exhibit high temperature superconductivity at moderate pressures. The Fm-3m phase of LaBeH8, with a fluorite-type H-Be alloy backbone, is predicted to be metastable and superconducting with a Tc ~ 191 K at 50 GPa; a substantially lower pressure than that required by the geometrically similar clathrate hydride LaH10 (170 GPa). Our approach paves the way for finding high-Tc ternary hydride superconductors at conditions close to ambient pressures.
2106.09879v2
2021-07-23
Favorable Interfacial Chemomechanics Enables Stable Cycling of High Li-Content Li-In/Sn Anodes in Sulfide Electrolyte Based Solid-State Batteries
Solid-state batteries (SSBs) can offer a paradigm shift in battery safety and energy density. Yet, the promise hinges on the ability to integrate high-performance electrodes with state-of-the-art solid electrolytes. For example, lithium (Li) metal, the most energy-dense anode candidate, suffers from severe interfacial chemomechanical issues that lead to cell failure. Li alloys of In/Sn are attractive alternatives, but their exploration has mostly been limited to the low capacity(low Li content)and In rich Li$_x$In (x$\leq$0.5). Here, the fundamental electro-chemo-mechanical behavior of Li-In and Li-Sn alloys of varied Li stoichiometries is unravelled in sulfide electrolyte based SSBs. The intermetallic electrodes developed through a controlled synthesis and fabrication technique display impressive (electro)chemical stability with Li$_6$PS$_5$Cl as the solid electrolyte and maintain nearly perfect interfacial contact during the electrochemical Li insertion/deinsertion under an optimal stack pressure. Their intriguing variation in the Li migration barrier with composition and its influence on the observed Li cycling overpotential is revealed through combined computational and electrochemical studies. Stable interfacial chemomechanics of the alloys allow long-term dendrite free Li cycling (>1000 h) at relatively high current densities (1 mA cm$^{-2}$) and capacities (1 mAh cm$^{-2}$), as demonstrated for Li$_{13}$In$_3$ and Li$_{17}$Sn$_4$, which are more desirable from a capacity and cost consideration compared to the low Li content analogues. The presented understanding can guide the development of high-capacity Li-In/Sn alloy anodes for SSBs.
2108.00843v1
2021-08-08
Reduced-Order Multiscale Modeling of Plastic Deformations in 3D Alloys with Spatially Varying Porosity by Deflated Clustering Analysis
Aluminum alloys are increasingly utilized as lightweight materials in the automobile industry due to their superior capability in withstanding high mechanical loads. A significant challenge impeding the large-scale use of these alloys in high-performance applications is the presence of manufacturing-induced, spatially varying porosity defects. In order to understand the impacts of these defects on the macro-mechanical properties of cast alloys, multiscale simulations are often required. In this paper, we introduce a computationally efficient reduced-order multiscale framework to simulate the behavior of metallic components containing process-induced porosity under irreversible nonlinear deformations. In our approach, we start with a data compression scheme that significantly reduces the number of unknown macroscale and microscale variables by agglomerating close-by finite element nodes into a limited number of clusters. Then, we use deflation methods to project these variables into a lower-dimensional space where the material elastoplastic behaviors are approximated. Finally, we solve for the unknown variables and map them back to the original, high-dimensional space. We call our method deflated clustering analysis and by comparing it to direct numerical simulations we demonstrate that it accurately captures macroscale deformations and microscopic effective responses. To illustrate the effect of microscale pores on the macroscopic response of a cast component, we conduct multi-scale simulations with spatially varying local heterogeneities that are modeled with a microstructure characterization and reconstruction algorithm.
2108.03742v4
2021-08-30
Co-deformation Between the Metallic Matrix and Intermetallic Phases in a Creep-Resistant Mg-3.68Al-3.8Ca Alloy
The microstructure of Mg-Al-Ca alloys consists of a hard intra- and intergranular eutectic Laves phase network embedded in a soft $\alpha$-Mg matrix. For such heterogeneous microstructures, the mechanical response and co-deformation of both phases under external load are not yet fully understood. We therefore used nano- and microindentation in combination with electron microscopy to study the deformation behaviour of an Mg-3.68Al-3.8Ca alloy. We found that the hardness of the Mg$_2$Ca phase was significantly larger than the $\alpha$-Mg phase and stays constant within the measured temperature range. The strain rate sensitivity of the softer $\alpha$-Mg phase and of the interfaces increased while activation volume decreased with temperature. The creep deformation of the Mg$_2$Ca Laves phase was significantly lower than the $\alpha$-Mg phase at 170 $^{\circ}$C. Moreover, the deformation zone around and below microindents depends on the matrix orientation and is influenced by the presence of Laves phases. Most importantly, slip transfer from the $\alpha$-Mg phase to the (Mg,Al)$_2$Ca Laves phase occurred, carried by the basal planes. Based on the observed orientation relationship and active slip systems, a slip transfer mechanism from the soft $\alpha$-Mg phase to the hard Laves phase is proposed. Further, we present implications for future alloy design strategies.
2108.13125v1
2021-09-05
Atomistic transport modeling, design principles and empirical rules for Low Noise III-V Digital Alloy Avalanche Photodiodes
A series of III-V ternary and quarternary digital alloy avalanche photodiodes (APDs) have recently been seen to exhibit very low excess noise. Using band inversion of an environment-dependent atomistic tight binding description of short period superlattices, we argue that a combination of increased effective mass, minigaps and band split-off are primarily responsible for the observed superior performance. These properties significantly limit the ionization rate of one carrier type, either holes or electrons, making the avalanche multiplication process unipolar in nature. The unipolar behavior in turn reduces the stochasticity of the multiplication gain. The effects of band folding on carrier transport are studied using the Non-Equilibrium Green's Function Method that accounts for quantum tunneling, and Boltzmann Transport Equation model for scattering. It is shown here that carrier transport by intraband tunneling and optical phonon scattering are reduced in materials with low excess noise. Based on our calculations, we propose five simple inequalities that can be used to approximately evaluate the suitability of digital alloys for designing low noise photodetectors. We evaluate the performance of multiple digital alloys using these criteria and demonstrate their validity.
2109.01995v1
2021-09-18
Efficiency and Forward Voltage of Blue and Green Lateral LEDs with V-shape defects and Random Alloy Fluctuation in Quantum Wells
For nitride-based blue and green light-emitting diodes (LEDs), the forward voltage $V_\text{for}$ is larger than expected, especially for green LEDs. This is mainly due to the large barriers to vertical carrier transport caused by the total polarization discontinuity at multiple quantum well and quantum barrier interfaces. The natural random alloy fluctuation in QWs has proven to be an important factor reducing $V_\text{for}$. However, this does not suffice in the case of green LEDs because of their larger polarization-induced barrier. V-defects have been proposed as another key factor in reducing $V_\text{for}$ to allow laterally injection into multiple quantum wells (MQWs), thus bypassing the multiple energy barriers incurred by vertical transport. In this paper, to model carrier transport in the whole LED, we consider both random-alloy and V-defect effects. A fully two-dimensional drift-diffusion charge-control solver is used to model both effects. The results indicate that the turn-on voltages for blue and green LEDs are both affected by random alloy fluctuations and V-defect density. For green LEDs, $V_\text{for}$ decreases more due to V-defects, where the smaller polarization barrier at the V-defect sidewall is the major path for lateral carrier injection. Finally, we discuss how V-defect density and size affects the results.
2109.08824v2
2021-09-29
Structure-property relations characterizing the devitrification of Ni-Zr glassy alloy thin films
The investigation of devitrification in thermally annealed nanodimensional glassy alloy thin films provides a comprehensive understanding of their thermal stability, which can be used to explore potential applications. The amorphous to crystalline polymorphous transformation of cosputtered NiZr alloy (Ni78Zr22 at%) films, with a thickness lower than the reported critical limit of devitrification, was studied through detailed structural characterization and molecular dynamics (MD) simulations. Devitrification to a nanocrystalline state (Ni7Zr2 structure) was observed at 800 degC, with an increase in density (approx 3.6%) much higher than that achieved in bulk alloys. Variation in the magnetic property of the films and the overall physical structure including morphology and composition were examined before and after annealing. MD simulations were employed to effectively elucidate not only the high densification but also the increased magnetic moment after annealing, which was correlated with the simulated change in the coordination number around Ni atoms. The structural relaxation process accompanying devitrification was described as a disorder-to-order transformation while highlighting the crucial role played by chemical short range order prevalent in glassy materials.
2109.14226v1
2021-09-30
On the influence of alloy composition on the additive manufacturability of Ni-based superalloys
The susceptibility of nickel-based superalloys to processing-induced crack formation during laser powder-bed additive manufacturing is studied. Twelve different alloys -- some of existing (heritage) type but also other newly-designed ones -- are considered. A strong inter-dependence of alloy composition and processability is demonstrated. Stereological procedures are developed to enable the two dominant defect types found -- solidification cracks and solid-state ductility dip cracks -- to be distinguished and quantified. Differential scanning calorimetry, creep stress relaxation tests at 1000$^\circ$C and measurements of tensile ductility at 800$^\circ$C are used to interpret the effects of alloy composition. A model for solid-state cracking is proposed, based on an incapacity to relax the thermal stress arising from constrained differential thermal contraction; its development is supported by experimental measurements using a constrained bar cooling test. A modified solidification cracking criterion is proposed based upon solidification range but including also a contribution from the stress relaxation effect. This work provides fundamental insights into the role of composition on the additive manufacturability of these materials.
2109.15274v1
2021-10-24
Isotropic finite-difference approximations for phase-field simulations of polycrystalline alloy solidification
Phase-field models of microstructural pattern formation during alloy solidification are commonly solved numerically using the finite-difference method, which is ideally suited to carry out computationally efficient simulations on massively parallel computer architectures such as Graphic Processing Units. However, one known drawback of this method is that the discretization of differential terms involving spatial derivatives introduces a spurious lattice anisotropy that can influence the solid-liquid interface dynamics. We find that this influence is significant for the case of polycrystalline dendritic solidification, where the crystal axes of different grains do not generally coincide with the reference axes of the finite-difference lattice. In particular, we find that with the commonly used finite-difference implementation of the quantitative phase-field model of binary alloy solidification, both the operating state of the dendrite tip and the dendrite growth orientation are strongly affected by the lattice anisotropy. To circumvent this problem, we use known methods in both real and Fourier space to derive finite-difference approximations of leading differential terms in 2D and 3D that are isotropic at order $h^2$ of the lattice spacing $h$. Importantly, those terms include the divergence of the anti-trapping current that is found to have a critical influence on pattern selection. The 2D and 3D discretizations use an approximated form of the anti-trapping current that facilitates the Fourier-space derivation of the associated isotropic differential operator at $O(h^2)$, but we also derive a 2D discretization of the standard form of this current. Finally, we present 2D and 3D phase-field simulations of alloy solidification, showing that the isotropic finite-difference implementations can dramatically reduce spurious lattice anisotropy effects.
2110.12448v1
2021-10-25
Atomistic mechanisms of binary alloy surface segregation from nanoseconds to seconds using accelerated dynamics
Although the equilibrium composition of many alloy surfaces is well understood, the rate of transient surface segregation during annealing is not known, despite its crucial effect on alloy corrosion and catalytic reactions occurring on overlapping timescales. In this work, CuNi bimetallic alloys representing (100) surface facets are annealed in vacuum using atomistic simulations to observe the effect of vacancy diffusion on surface separation. We employ multi-timescale methods to sample the early transient, intermediate, and equilibrium states of slab surfaces during the separation process, including standard MD as well as three methods to perform atomistic, long-time dynamics: parallel trajectory splicing (ParSplice), adaptive kinetic Monte Carlo (AKMC), and kinetic Monte Carlo (KMC). From nanosecond (ns) to second timescales, our multiscale computational methodology can observe rare stochastic events not typically seen with standard MD, closing the gap between computational and experimental timescales for surface segregation. Rapid diffusion of a vacancy to the slab is resolved by all four methods in tens of ns. Stochastic re-entry of vacancies into the subsurface, however, is only seen on the microsecond timescale in the two KMC methods. Kinetic vacancy trapping on the surface and its effect on the segregation rate are discussed. The equilibrium composition profile of CuNi after segregation during annealing is estimated to occur on a timescale of seconds as determined by KMC, a result directly comparable to nanoscale experiments.
2110.13249v1
2021-11-10
In-situ measurements of dendrite tip shape selection in a metallic alloy
The size and shape of the primary dendrite tips determine the principal length scale of the microstructure evolving during solidification of alloys. In-situ X-ray measurements of the tip shape in metals have been unsuccessful so far due to insufficient spatial resolution or high image noise. To overcome these limitations, high-resolution synchrotron radiography and advanced image processing techniques are applied to a thin sample of a solidifying Ga-35wt.%In alloy. Quantitative in-situ measurements are performed of the growth of dendrite tips during the fast initial transient and the subsequent steady growth period, with tip velocities ranging over almost two orders of magnitude. The value of the dendrite tip shape selection parameter is found to be $\sigma^* = 0.0768$, which suggests an interface energy anisotropy of $\varepsilon_4 = 0.015$ for the present Ga-In alloy. The non-axisymmetric dendrite tip shape amplitude coefficient is measured to be $A_4 \approx 0.004$, which is in excellent agreement with the universal value previously established for dendrites.
2111.05658v4
2021-11-22
Nucleation-growth versus spinodal decomposition in Fe-Cr alloys: an experimental verification by atom probe tomography and small angle neutron scattering
Identifying the operative mode of phase separation (spinodal decomposition (SD) or nucleation-growth (NG)) remains a largely unexplored area of research in spite of its importance. The present work examines this critically in Fe-Cr system using atom probe tomography (APT) and small angle neutron scattering (SANS), and establishes the framework to distinguish the two different modes of alpha-prime phase separation in thermally aged Fe-35 at.% Cr and Fe-20 at.% Cr alloys. Independent APT analysis determines the mode of phase separation on the basis of: (i) presence / absence of periodic chemical fluctuation through radial distribution function analysis; and (ii) inter-phase interface characteristics (diffuse / sharp). SANS analysis, in contrast, yields virtually indistinguishable correlation peaks for both the modes, which necessitates further investigation of the several different aspects of SANS profiles in the light of APT results. For the first time, key features of SANS profiles have been identified that can unambiguously distinguish SD from NG in Fe-Cr system: (i) nature of temporal evolution of FWHM of the correlation peak; and (ii) appropriate value of 'gamma' for fitting with the dynamic scaling model ('gamma'= 6 for SD, Fe-35 at.% Cr alloy; 'gamma'= 4 for NG, Fe-20 at.% Cr alloy).
2111.11340v1
2021-12-22
Graphene Layer Morphology as an Indicator of the Metals Alloy Formation at the Interface
The intercalation of different species in graphene-metal interfaces is widely used to stabilise the artificial phases of different materials. However, formation of the surface alloys upon the guest-metal intercalation is still an open question, which is very important for the fabrication of graphene-based interfaces with desired properties. Here, the widely studied interfaces of graphene with Ru(0001) and Ir(111) were modified using intercalation of a thin Mn layer and investigated by means of scanning tunnelling microscopy (STM) accompanied by density functional theory (DFT) calculations, which reproduce the observed experimental data. It is found that Mn forms a pseudomorphic layer on Ru(0001) under a strongly buckled graphene layer. In case of Mn intercalation in graphene/Ir(111), a buried thin layer of MnIr alloy is formed beneath the first Ir layer under a flat graphene layer. This unexpected observation is explained on the basis of phase diagram pictures for the Mn-Ru and Mn-Ir systems as well as via comparison of calculated total energies for the respective interfaces. Our results shed light on the understanding of mechanisms of the alloys formation at the graphene-metal interfaces and demonstrate their potential for the preparation of tailored interfaces for future graphene-based applications.
2112.13733v1
2022-05-11
Correlated subgrain and particle analysis of a recovered Al-Mn alloy by directly combining EBSD and backscatter electron imaging
Correlated analysis of (sub)grains and particles in alloys is important to understand transformation processes and control material properties. A multimodal data fusion workflow directly combining subgrain data from electron backscatter diffraction (EBSD) and particle data from backscatter electron (BSE) images in the scanning electron microscope is presented. The BSE images provide detection of particles smaller than the applied step size of EBSD down to 0.03 $\mu$m in diameter. The workflow is demonstrated on a cold-rolled and recovered Al-Mn alloy, where constituent particles formed during casting and dispersoids formed during subsequent heating affect recovery and recrystallization upon annealing. The multimodal dataset enables statistical analysis including subgrains surrounding constituent particles and dispersoids' location with respect to subgrain boundaries. Among the subgrains of recrystallization texture, Cube{001}$\left<100\right>$ subgrains experience an increased Smith-Zener drag from dispersoids on their boundaries compared to CubeND{001}$\left<310\right>$ and P{011}$\left<\bar{5}\bar{6}6\right>$ subgrains, with the latter experiencing the lowest drag. Subgrains at constituent particles are observed to have a growth advantage due to a lower dislocation density and higher boundary misorientation angle. The dispersoid size per subgrain boundary length increases as a function of misorientation angle. The workflow should be applicable to other alloy systems where there is a need for analysis correlating grains and grain boundaries with secondary phases smaller than the applied EBSD step size but resolvable by BSE imaging.
2205.05514v2
2022-06-01
Non-equilibrium magnetic response in concentrated spin-glass AuFe(11%) alloy
We report a detailed study of dc magnetization and ac susceptibility performed on the zero field cooled (ZFC) and field cooled (FC) state of polycrystalline AuFe(11%) alloy. The temperature variation of ZFC and FC dc magnetization at low fields show a distinct peak around Tf = 33 K, which indicates the cooperative freezing of the finite size spin clusters. A weak thermomagnetic irreversibility between ZFC and FC magnetization appears at a temperature Tir, which is slightly below Tf. The ZFC ac susceptibility shows a sharp cusp at Tf, which shifts towards higher temperatures with an increase in the frequency of the ac magnetic field. When ac susceptibility is recorded after cooling the sample from high temperature in the presence of dc bias magnetic field, the susceptibility cusp gets broadened. In this case, no perceptible frequency dependency of the Tf has been observed, but a significant dispersion in the ac susceptibility is present below Tf. This clearly indicates the non-equilibrium nature of the FC state.In addition, the FC state of AuFe(11%) alloy exhibits a pronounced memory effect which further underlines that the FC state is not an equilibrium state. In contrast to the general perception obtained through the meanfield theories of thermodynamic phase transition in spin-glass envisaging the FC state to be an equilibrium state, the present experimental results clearly indicate that the energy landscape of the FC state of AuFe(11%) alloy is a nontrivial one
2206.00286v1
2022-07-04
Dielectric function of CuBr$_\mathrm{x}$I$_{1-\mathrm{x}}$ alloy thin films
We study the dielectric function of CuBr$_\mathrm{x}$I$_{1-\mathrm{x}}$ thin film alloys using spectroscopic ellipsometry in the spectral range between 0.7 eV to 6.4 eV, in combination with first-principles calculations based on density functional theory. Through the comparison of theory and experiment, we attribute features in the dielectric function to electronic transitions at specific k-points in the Brillouin zone. The observed bandgap bowing as a function of alloy composition is discussed in terms of different physical and chemical contributions. The band splitting at the top of the valence band due to spin-orbit coupling is found to decrease with increasing Br-concentration, from a value of 660 meV for CuI to 150 meV for CuBr. This result can be understood considering the contribution of copper d-orbitals to the valence band maximum as a function of the alloy composition.
2207.01344v2
2022-07-11
Physics-Based Machine-Learning Approach for Modeling the Temperature-Dependent Yield Strengths of Medium- or High-Entropy Alloys
Machine learning is becoming a powerful tool to predict temperature-dependent yield strengths (YS) of structural materials, particularly for multi-principal-element systems. However, successful machine-learning predictions depend on the use of reasonable machine-learning models. Here, we present a comprehensive and up-to-date overview of a bilinear log model for predicting temperature-dependent YS of medium-entropy or high-entropy alloys (MEAs or HEAs). In this model, a break temperature, Tbreak, is introduced, which can guide the design of MEAs or HEAs with attractive high-temperature properties. Unlike assuming black-box structures, our model is based on the underlying physics, incorporated in form of a priori information. A technique of global optimization is employed to enable the concurrent optimization of model parameters over low- and high-temperature regimes, showing that the break temperature is consistent across YS and ultimate strength for a variety of HEA compositions. A high-level comparison between YS of MEAs/HEAs and those of nickel-based superalloys reveal superior strength properties of selected refractory HEAs. For reliable operations, the temperature of a structural component, such as a turbine blade, made from refractory alloys may need to stay below Tbreak. Once above Tbreak, phase transformations may start taking place, and the alloy may begin losing structural integrity.
2207.05171v1
2022-07-28
Evolution of short-range magnetic correlations in ferromagnetic Ni-V alloys
We experimentally study how the magnetic correlations develop in a binary alloy close to the ferromagnetic quantum critical point with small-angle neutron scattering (SANS). Upon alloying the itinerant ferromagnet nickel with vanadium, the ferromagnetic order is continuously suppressed. The critical temperature Tc vanishes when vanadium concentrations reach the critical value of xc=0.116 indicating a quantum critical point separating the ferromagnetic and paramagnetic phases. Earlier magnetization and $\mu$SR data have indicated the presence of magnetic inhomogeneities in Ni(1-x)V(x) and, in particular, recognize the magnetic clusters close to xc, on the paramagnetic and on the ferromagnetic sides with nontrivial dynamical properties [R. Wang et al., Phys. Rev. Lett. 118, 267202 (2017)]. We present the results of SANS study with full polarization analysis of polycrystalline Ni(1-x)V(x) samples with x=0.10 and x=0.11 with low critical temperatures Tc below 50 K. For both Ni-V samples close to xc we find isotropic magnetic short-range correlations in the nanometer-scale persisting at low temperatures. They are suppressed gradually in higher magnetic fields. In addition, signatures of long-range ordered magnetic domains are present below Tc. The fraction of these magnetic clusters embedded in the ferromagnetic ordered phase grows towards xc and agrees well with the cluster fraction estimate from the magnetization and $\mu$SR data. Our SANS studies provide new insights into the nature of the inhomogeneities in a ferromagnetic alloy close to a quantum critical point.
2207.14196v2
2022-08-11
Quantitative assessment of the microstructural factors controlling the fatigue crack initiation mechanisms in AZ31 Mg alloy
The deformation and fatigue crack nucleation mechanisms were studied by means of slip trace analysis and secondary electron microscopy in a textured AZ31B-O Mg alloy subjected to fully-reversed cyclic deformation at two different cyclic strain semi-amplitudes. Samples were deformed in two orientations leading to symmetric and non-symmetric cyclic stress-strain curves due to the activation of different deformation mechanisms. They were ascertained in longitudinal sections of the specimens, which included a large number of grains (from 1500 to 4500 for each specimen), to obtain statistically significant results. If the dominant deformation mechanisms were basal slip and tensile twinning/detwinning, the most damaging fatigue cracks were nucleated along twins in large grains, together with cracks parallel to basal slip bands associated with the localization of deformation in clusters of small grains suitably oriented for basal slip. If the main deformation mechanisms were tensile twinning/detwinning and pyramidal slip, the longest fatigue cracks were nucleated along pyramidal slip bands in large grains. Grain boundary cracks around small grains were found in all cases, but they were not critical from the viewpoint of fatigue failure. This information is relevant to assess the effect of the microstructural features on the fatigue life of Mg alloys and as input to simulate the fatigue behavior of Mg alloys using fatigue indicator parameters.
2208.05861v1
2022-09-13
Strain and composition dependencies of the near bandgap optical transitions in monoclinic (Al$_x$Ga$_{1-x}$)$_2$O$_3$ alloys with coherent biaxial in-plane strain on (010) Ga$_2$O$_3$
The bowing of the energy of the three lowest band-to-band transitions in $\beta$-(Al$_{x}$Ga$_{1-x}$)$_2$O$_3$ alloys was resolved using a combined density functional theory (DFT) and generalized spectroscopic ellipsometry (GSE) approach. The DFT calculations of the electronic band structure of both, $\beta$-Ga$_2$O$_3$ and $\theta$-Al$_2$O$_3$, allow extracting of the linear portion of the energy shift in the alloys, and provide a method for quantifying the role of coherent strain present in the $\beta$-(Al$_{x}$Ga$_{1-x}$)$_2$O$_3$ thin films on (010) $\beta$-Ga$_2$O$_3$ substrates. The energies of band-to-band transitions were obtained using the spectroscopic ellipsometry eigenpolarization model approach [A. Mock et al., Phys. Rev. B 95, 165202 (2017)]. After subtracting the effects of strain which also induces additional bowing and after subtraction of the linear portion of the energy shift due to alloying, the bowing parameters associated with the three lowest band-to-band transitions in monoclinic $\beta$-(Al$_{x}$Ga$_{1-x}$)$_2$O$_3$ are found.
2209.06025v1
2022-11-15
Enhanced piezoelectric response of AlN via alloying of transitional metals, and influence of type and distribution of transition metals
Aluminum nitride (AlN) is an important piezoelectric material for a wide range of applications, many efforts are devoted to improving its piezoelectric response by alloying with transition metals (TMs). In this paper, the influence of the type and distribution of TM on the piezoelectric response is discussed for the first time. TM0.0625Al0.9375N with twenty-eight different TMs are investigated, and most show higher values of piezoelectric strain modulus d33 than that of AlN. This is because the TM introduces weaker TM-N bonds and locates closer to the centre of three neighbouring N atoms. The location of TM is determined to be significantly correlated with its group number. Alloys of TMxAl1-xN (TM=Sc, Cr, Sr, Mo, Ru and Rh) with varying x are further studied. On basis of the cost of the TMs and piezoelectric performances, the alloy with Mo is more effective in enhancing d33. A high d33 of 12.3 times that of pure AlN is realized in a metastable configuration of Mo0.167Al0.833N. The distribution of Mo plays a key role in the piezoelectric performance. A higher d33 is more likely to appear in MoxAl1-xN with more Al sublayers containing Mo atoms and with fewer dimers of Mo atoms along the z-axis.
2211.07870v1
2022-12-16
Compositional phase stability in medium-entropy and high-entropy Cantor-Wu alloys from an ab initio all-electron, Landau-type theory and atomistic modelling
We describe implementation and analysis of a first-principles theory, derived in an earlier work, for the leading terms in an expansion of a Gibbs free energy of a multi-component alloy in terms of order parameters that characterize potential, compositional phases. The theory includes effects of rearranging charge and other electronics from changing atomic occupancies on lattice sites. As well as the rigorous description of atomic short-range order in the homogeneously disordered phase, pairwise interaction parameters suited for atomistic modelling in a multicomponent setting can be calculated. From our study of an indicative series of the Cantor-Wu alloys, NiCo, NiCoCr, NiCoFeCr, and NiCoFeMnCr, we find that the interactions are not approximated well either as pseudobinary or restricted to nearest neighbour range. Our computed order-disorder transition temperatures are low, consistent with experimental observations, and the nature of the ordering is dominated by correlations between Ni, Co, and Cr, while Fe and Mn interact weakly. Further atomistic modelling suggests that there is no true single-phase low-temperature ground state for these multicomponent systems. Instead the single-phase solid solution is kept stable to low temperatures by the large configurational entropy and the Fe, Mn dilution effects. The computationally cost-effectiveness of our method makes it a good candidate for further exploration of the space of multicomponent alloys.
2212.08468v1
2022-12-21
Effect of Ti addition on the structural, thermodynamic, and elastic properties of Ti$_{x}$(HfNbTaZr)$_{(1-x)/4}$ alloys
The structure and thermodynamic properties of Ti$_x$(HfNbTaZr)$_{(1-x)/4}$ from Refractory High Entropy multicomponent Alloys to pure titanium are investigated employing comprehensive MCSQS realizations of the disordered atomic structure and DFT calculations. We showed that to model the random structure in a limited supercell, it is necessary to probe a large space of random configurations with respect to the nearest neighbor's shells. Mimicking the randomness with the many-body terms does not lead to significant improvements in the mixing energy, but modeling the random structure with the few nearest neighbor pairs leads to improvements in the mixing energy. Furthermore, we demonstrated the existence of weak to medium SRO for the two equimolar compositions. Chemical ordering is investigated by associating a large number of MCSQS realizations to DFT energy calculations, and SRO results are rationalized in terms of the crystallographic structure of the pairs of elements and binary phase diagrams. When Ti is added to Ti$_x$(HfNbTaZr)$_{(1-x)/4}$ alloys, the mixing energy remains slightly positive for all $x$. For $x$ > 0.4, a phase transition in favor of an hcp structure is observed in agreement with the predictions of the Bo-Md diagram. At $x$ = 0.5, a dual phase is predicted. Ti content in this class of alloys could be a practical way to select phase structure and tailor the elastic properties to specific applications.
2212.10977v3
2023-01-06
APC Nb$_3$Sn superconductors based on internal oxidation of Nb-Ta-Hf alloys
In the last few years, a new type of Nb$_3$Sn superconducting composite, containing a high density of artificial pinning centers (APC) generated via an internal oxidation approach, has demonstrated a significantly superior performance relative to present, state-of-the-art commercial Nb$_3$Sn conductors. This was achieved via the internal oxidation of Nb-4at.%Ta-1at.%Zr alloy. On the other hand, our recent studies have shown that internal oxidation of Nb-Ta-Hf alloys can also lead to dramatic improvements in Nb$_3$Sn performance. In this work we follow up this latter approach, fabricating a 61-stack APC wire based on the internal oxidation of Nb-4at.%Ta-1at.%Hf alloy, and compare its critical current density (Jc) and irreversibility field (Birr) with APC wires made using Nb-4at.%Ta-1at.%Zr. A second goal of this work was to improve the filamentary design of APC wires in order to improve their wire quality and electromagnetic stability. Our new modifications have led to significantly improved RRR and stability in the conductors, while still keeping non-Cu Jc at or above the FCC Jc specification. Further improvement via optimization of the wire recipe and design is ongoing. Finally, additional work needed to make APC conductors ready for applications in magnets is discussed.
2301.02571v2
2023-01-10
Geometric Study on Canonical Nonlinearity for FCC-based Binary Alloys
For classical discrete systems under constant composition (typically reffered to as substitutional alloys), canonical average phi typically provides a complicated nonlinear map from a set of potential energy surface to that of macroscropic structure in thermodynamic equilibrium, the so-called canonical nonlinearity: CN. Although our recent study reveals that the CN can be reasonablly addressed for individual microscopic configuration by two different ways of special vector field on configuration space, anharmonicity in the structural degree of freedoms (ASDF), and Kullback-Leibler (KL) divergence DKL, that is the conceptual extention of ASDF to statistical manifold to include further non-local information about CN, their direct correlation on real lattices, is still totally unclear. We here tuckle this problem for fcc-based equiatomic binary alloys that have been most studied in the CN-based context. We confirm that while one of the contribution to CN of DdG for each configuration, due to difference in CDOS from Gaussian, exhibits significant positive correlation with ASDF, another contribution of Dns due to non-separability in structural degee of freedoms (SDFs) exhibit no effective correlation with ASDF, which can be naturally accepted since the former contribution depends on ASDF itself, while the latter is independent. We find that average of Dns over all configurations for sets of SDFs can be well-characterized by information about asymmetric Hausdorff distance between configurational polyhedra (CP) for practical and ideally separable system, and CP hypervolumes. This fact certainly indicates that non-local information about CN has profound connection to the geometric configuration for ground-state structures of alloys on configuration space.
2301.03741v2
2023-01-12
Effect of hydrostatic pressure and alloying on thermoelectric properties of van der Waals solid KMgSb: An \textit{ab-initio} study
Through a combined first-principles and Boltzmann transport theory, we systematically investigate the thermal and electrical transport properties of the unexplored ternary quasi two-dimensional KMgSb system of KMgX (X = P, As, Sb, and Bi) family. Herein, the transport properties of KMgSb under the application of hydrostatic pressure and alloy engineering are reported. At a carrier concentration of $\sim8\times10^{19}~\mathrm{cm^{-3}}$, the figure of merit zT ($\sim0.75$) for both the $n$-type and $p$-type of KMgSb closely matched, making it an attractive option for engineering both legs of a thermoelectric device using the same material. This is particularly desirable for high-performance thermoelectric applications. Furthermore, the zT value increases as pressure decreases, further enhancing its potential for use in thermoelectric devices. In the case of substitutional doping (replacing 50 \% Sb by Bi atom), we observed $\sim49~\%$ (in-plane) increase in the peak thermoelectric figure of merit (zT). The maximum zT value obtained after alloy engineering is $\sim1.45$ at 900~K temperature. Hydrostatic pressure is observed to be a great tool to tune the lattice thermal conductivity ($\kappa_L$). We observed that the negative pressure-like effects could be achieved by chemically doping bigger-size atoms, especially when $\kappa_L$ is a property under investigation. Through our computational investigation, we explain that hydrostatic pressure and alloy engineering may improve thermoelectric performance dramatically.
2301.04969v2
2023-03-18
Rate dependence of damage formation in metallic-intermetallic Mg-Al-Ca composites
We study a cast Mg-4.65Al-2.82Ca alloy with a microstructure containing $\alpha$-Mg matrix reinforced with a C36 Laves phase skeleton. Such ternary alloys are targeted for elevated temperature applications in automotive engines since they possess excellent creep properties. However, in application, the alloy may be subjected to a wide range of strain rates and in material development, accelerated testing is often of essence. It is therefore crucial to understand the effect of such rate variations. Here, we focus on their impact on damage formation. Due to the locally highly variable skeleton forming the reinforcement in this alloy, we employ an analysis based on high resolution panoramic imaging by scanning electron microscopy coupled with automated damage analysis by deep learning-based object detection and classification convolutional neural network algorithm (YOLOV5). We find that with decreasing strain rate the dominant damage mechanism for a given strain level changes: at a strain rate of $5\cdot10^{-4}/s$ the evolution of microcracks in the C36 Laves phase governs damage formation. However , when the strain rate is decreased to $5\cdot10^{-6}/s$, interface decohesion at the $\alpha$-Mg/Laves phase interfaces becomes equally important. We also observe a change in crack orientation indicating an increasing influence of plastic co-deformation of the {\alpha}-Mg matrix and Laves phase. We attribute this transition in leading damage mechanism to thermally activated processes at the interface.
2303.10477v1
2023-03-25
Prediction of novel final phases in aged uranium-niobium alloys
Ordered intermetallics are long believed to be the final products of the aging of U-Nb solid solutions at low temperatures, a crucial property for the practical applications of this alloy in engineering and industry. However, such conjectured ordered compounds have not been experimentally or theoretically established. Herein, numerical evidence for ordered intermetallic U-Nb compounds is presented using thorough first-principles structure predictions up to 500 GPa. Two stable U2Nb compounds and one metastable U2Nb and one metastable U3Nb were discovered. A unique hybridized transition driven by pressure was observed in U2Nb, which is a superposition of one first-order transition and another second-order transition, leading to striking features near the transition pressure of 21.6 GPa. The decomposition limit of these compounds at high temperature was also investigated. The strong stability of U2Nb in the region of low pressure and high temperature was revealed. This discovery of ordered U2Nb and its strong stability over a wide pressure range completely changed the phase diagram of U-Nb alloys and shed new light on the dynamic response and aging mechanism of U-Nb alloys.
2303.14442v1
2023-03-27
Microstructural engineering by heat treatments of multi-principal element alloys via spinodal mediated phase transformation pathways
Nanoscale multi-phase microstructures observed in multi-principal element alloys (MPEAs) such as $\rm AlMo_{0.5}NbTa_{0.5}TiZr$, $\rm Al_{0.5}NbTa_{0.8}Ti_{1.5}V_{0.2}Zr$, $\rm TiZrNbTa$, $\rm AlCoCrFeNi$ and $\rm Fe_{15}Co_{15}Ni_{20}Mn_{20}Cu_{30}$ that exhibit promising mechanical or functional properties may have evolved through spinodal-mediated phase transformation pathways (PTPs). The microstructures in such MPEA systems could be further engineered for targeted applications by appropriately designing the alloy composition and heat-treatment schedule. In this study, we investigate systematically how different heat treatment schedules such as single-step isothermal aging, two-step isothermal aging and continuous cooling alter the interplay among the various factors associated with alloy composition, such as volume fraction of individual phases, lattice misfit and modulus mismatch between the co-existing phases. We have determined the degree to which these factors influence significantly the spinodal-mediated PTPs and the corresponding microstructures by use of high-throughput phase-field simulations. In particular, we demonstrate that the microstructural topology (i.e., which phase forms the continuous matrix and which phase forms discrete precipitates) in the same MPEA having an asymmetric miscibility gap could be inverted simply by a continuous cooling heat treatment. Further, we reveal a rich variety of novel hierarchical microstructures that could be designed using two-step isothermal aging heat treatments in MPEA systems with symmetric or asymmetric miscibility gaps. These simulation results may shed light on novel microstructure design and engineering for the above-mentioned MPEA systems.
2303.15370v2
2023-05-09
Interaction of $\langle a \rangle$ prismatic screw dislocations with the $α-β$ interface side face in $α-β$ Ti alloys
Slip transmission across $\alpha-\beta$ interfaces is of great significance in understanding the strength of $\alpha-\beta$ Ti alloys for aerospace applications. Molecular statics (MS) and molecular dynamics (MD) simulations were conducted to investigate the mechanisms of slip transmission of $\langle a \rangle$ prismatic screw dislocations across the $\alpha-\beta$ interface side face. In these simulations, the $\alpha$ phase consisted of pure HCP Ti whereas the $\beta$ phase was modeled as Ti$_{60}$Nb$_{40}$ BCC random alloy using a Ti-Nb interatomic potential. Firstly, the misfit dislocations structure on the $\alpha-\beta$ interface side face has been characterized from MS simulations. This predicted dislocation structure is in good agreement with experimental observations in Ti-alloys. Secondly, MD simulations of the interaction of $[a_1]$, $[a_2]$, and $[a_3]$ prismatic screw dislocations with the interface side face in an $\alpha-\beta$ bi-crystal were performed at different temperatures. A distinct barrier of the interface side face to different types of dislocation transmission was found. The origin of this anisotropy in the slip transmission is due to the relative misalignment of the slip systems between the $\alpha$ and the $\beta$ phases from the Burgers orientation relationship. Finally, the mechanisms of slip transmission of each dislocation type were analyzed in a detailed atomistic description and compared to experimental observations.
2305.05737v2
2023-05-10
Local Alloy Order in a Ge1-xSnx/Ge Epitaxial Layer
The local ordering of atoms in alloys directly has a strong impact on their electronic and optical properties. This is particularly relevant in nonrandom alloys, especially if they are deposited using far from the equilibrium processes, as is the case of epitaxial Ge1-xSnx layers. In this work, we investigate the arrangement of Ge and Sn atoms in optoelectronic grade Ge1-xSnx epitaxial layers featuring a Sn content in the 5-14% range by using polarization-dependent Raman spectroscopy and density-functional-theory calculations. The thorough analysis of the polarization-dependent spectra in parallel and perpendicular configuration allowed us to properly tag all the observed vibrational modes, and to shed light on that associated to disorder-assisted Raman transitions. Indeed, with the help of large-scale atomistic simulations, we were able to highlight how the presence of Sn atoms, that modify the local environments of Ge atoms, gives rise to two spectral features at different Raman shifts, corresponding to distortions of the atomic bonds. This analysis provides a valuable framework for advancing the understanding of the vibrational properties in Ge1-xSnx alloys, particularly with regard to the impact of local ordering of the different atomic species.
2305.06005v2
2023-05-25
Bandgap manipulation of hBN by alloying with aluminum: absorption properties of hexagonal BAlN
The versatile range of applications for two-dimensional (2D) materials has encouraged scientists to further engineer the properties of these materials. This is often accomplished by stacking layered materials into more complex van der Waals heterostructures. A much less popular but technologically promising approach is the alloying of 2D materials with different element compositions. In this work, we demonstrate a first step in manipulating the hBN bandgap in terms of its width and indirect/direct character of the optical transitions. We present a set of aluminum alloyed hexagonal boron nitride (hBAlN) samples that were grown by metal organic vapor phase epitaxy (MOVPE) on 2-inch sapphire substrates with different aluminum concentration. Importantly, the obtained samples revealed a sp$^2$-bonded crystal structure. Optical absorption experiments disclosed two strong peaks in the excitonic spectral range with absorption coefficient $\alpha \sim 10^6$ cm$^{-1}$. Their energies correspond very well with the energies of indirect and direct bandgap transitions in hBN. However, they are slightly redshifted. This observation is in agreement with predictions that alloying with Al leads to a decrease of the bandgap energy. The observation of two absorption peaks can be explained in terms of mixing electronic states in the K and M conduction band valleys, which leads to a significant enhancement of the absorption coefficient for indirect transitions.
2305.15810v1
2023-07-08
Towards reducing tension-compression yield and cyclic asymmetry in pure magnesium and magnesium-aluminum alloy with cerium addition
In this study, we report the effect of cerium (Ce) addition on the tension-compression yield and cyclic asymmetry in commercially pure magnesium (Cp-Mg) and Mg-Al alloy at room temperature (RT). The investigated materials Cp-Mg, Mg-0.5Ce, and Mg-3Al-0.5Ce were extruded at 400{\deg}C, followed by annealing at the same temperature for one hour. Incorporating 0.5wt.% Ce in pure Mg results in the weakening of its basal texture, uniform distribution of Mg12Ce precipitates, and grain size refinement. Consequently, the tensile yield strength and ductility of pure Mg increased, and tension-compression yield asymmetry was eliminated. However, the presence of 3wt.% Al in Mg suppresses the beneficial effects of Ce addition. The formation of complex precipitates, such as Mg-Al-Ce and Al11Ce3, limits the weakening of the basal texture, reduction in grain size, improvement in ductility, and elimination of tension-compression yield asymmetry observed in Mg-0.5Ce. Nevertheless, Al contributes to the solid solution strengthening in Mg and possibly lowers the critical stress required for twinning in Mg, resulting in the highest tensile strength of Mg-3Al-0.5Ce. Finally, the addition of 0.5wt.% Ce enhances the cyclic strength, stabilizes cyclic stress response, reduces inelastic strain, and minimizes cyclic asymmetry in both pure Mg and Mg-Al alloy while maintaining a comparable fatigue life. Overall, Ce addition positively impacts the microstructure and mechanical behavior of pure Mg and its investigated alloy. The reasons for these improvements are discussed in detail.
2307.04051v3
2023-07-15
Exploring the Impact of Configurational Entropy on the Design and Development of CoNi-Based Superalloys for Sustainable Applications
A comprehensive literature review on recently rediscovered Co- and/or CoNi-based superalloys, strengthened by the {\gamma}' phase, revealed a relationship between the configurational entropy of the system and the {\gamma}' solvus temperature. This study was conducted on a high Cr CoNi-based superalloy system with high configurational entropy to test our hypothesis based on the sustainable metallurgy framework. Thermodynamic calculations were performed to design the chemical compositions, followed by vacuum casting and heat treatments to produce the desired alloys. The microstructures were characterized using a scanning electron microscope, electron backscattered diffraction, transmission electron microscope, and differential thermal analysis. Microhardness and nanoindentation tests were employed to measure the mechanical properties. The results showed that both the configurational entropy and the type of alloying elements determine the final high-temperature performance of the alloys. We found that to enhance the higher {\gamma}' solvus temperature, the configurational entropy should be increased by adding {\gamma}' stabilizing elements. The microstructural and mechanical characteristics of the designed alloys before and after heat treatments are discussed in detail. The outcome of this study is beneficial for developing cobalt-based high-entropy superalloys with appropriate processing windows and freezing ranges for advanced sustainable manufacturing purposes, such as using powder bed fusion technologies.
2307.07731v1
2023-08-10
Exploring Solute Behavior and Texture Selection in Magnesium Alloys at the Atomistic Level
This study advances our understanding of how chemical binding and solute distribution impact grain boundary segregation behavior and subsequent annealing texture modification in lean Mg-X-Zn alloys (X = RE or Ca). Notably, differences in Ca and Gd solute behavior at grain boundaries were revealed, where Ca exhibited stronger binding to vacancy sites than Gd, resulting in elevated Ca segregation and an RD-TD-type texture. The introduction of Zn showed significant synergistic effects on solute clustering, with Gd-Zn pairs forming more favorably than Ca-Zn pairs, leading to a strong synergy between Zn and Gd. This promoted their co-segregation and high concentration at the grain boundary, generating a unique TD-spread texture. In contrast, weaker binding in Ca-Zn pairs did not affect Ca segregation but influenced Zn segregation, which underscores the importance of solute binding behavior in alloy design concepts. Additionally, the combined atomicscale experiments and ab initio predictions provide strong evidence that selective texture development in Mg alloys is tied to heterogeneous solute-boundary interactions, where the sensitivity of the binding energy to volumetric strain affects solute segregation at grain boundaries, resulting in varying grain boundary mobilities and specific texture component growth. It also emphasizes that solute behavior in clustering and segregation is influenced not only by atomic size but also by chemical binding strength with vacancies or co-added Zn.
2308.05811v2
2023-08-17
On the role of selective nucleation and growth to recrystallization texture development in a Mg-Gd-Zn alloy
One of the main material properties altered by rare earth additions in magnesium alloys is texture, which can be specifically adjusted to enhance ductility and formability. The current study aims at illuminating the texture selection process in a Mg-0.073at%Gd-0.165at%Zn alloy by investigating recrystallization nucleation and early nucleus growth during static recrystallization. An as-cast sample of the investigated alloy was deformed in uniaxial compression at 200{\deg}C till 40% strain and was then cut into two halves for subsequent microstructure characterization via ex-situ and quasi in-situ EBSD investigations. In order to gain insights into the evolution of texture during recrystallization, the contributions from dynamic and static recrystallization were initially separated and the origin of the non-basal orientation of recrystallization nuclei was traced back to several potential nucleation sites within the deformed matrix. Considering the significant role of double-twin band recrystallization in determining the recrystallization texture, this type of recrystallization nucleation was further investigated via quasi-in-situ EBSD on a deformed sample, annealed at 400{\deg} for different annealing times. With progressive annealing a noticeable trend was observed, in which the basal nuclei gradually diminished and eventually vanished from the annealed microstructure. In contrast, the off-basal nuclei exhibited continuous growth, ultimately becoming the dominant contributors to the recrystallization texture. The study therefore emphasizes the importance of particular nucleation sites that generate favorably oriented off-basal nuclei, which over the course of recrystallization outcompete the neighboring basal-oriented nuclei in terms of growth, and thereby dominate the recrystallization texture.
2308.08916v1
2023-08-28
Defects and Oxygen Impurities in Ferroelectric Wurtzite Al$_{1-x}$Sc$_x$N Alloys
III-nitrides and related alloys are widely used for optoelectronics and as acoustic resonators. Ferroelectric wurtzite nitrides are of particular interest because of their potential for direct integration with Si and wide bandgap semiconductors, and unique polarization switching characteristics; such interest has taken off since the first report of ferroelectric Al$_{1-x}$Sc$_x$N alloys. However, the coercive fields needed to switch polarization are on the order of MV/cm, which is 1-2 orders of magnitude larger than oxide perovskite ferroelectrics. Atomic-scale point defects are known to impact the dielectric properties, including breakdown fields and leakage currents, as well as ferroelectric switching. However, very little is known about the native defects and impurities in Al$_{1-x}$Sc$_x$N, and their effect on the dielectric properties. In this study, we use first-principles calculations to determine the formation energetics of native defects and unintentional oxygen incorporation in Al$_{1-x}$Sc$_x$N. We find that nitrogen vacancies are the dominant native defects, and that they introduce multiple mid-gap states that can lead to premature dielectric breakdown in ferroelectrics and carrier recombination in optoelectronics. Growth under N-rich conditions will reduce the concentration of these deep defects. We also investigate unintentional oxygen incorporation on the nitrogen site and find that the substitutional defect is present in high concentrations, which can contribute to increased temperature-activated leakage currents. Our findings provide fundamental understanding of the defect physics in Al$_{1-x}$Sc$_x$N alloys, which is critical for future deployment of ferroelectric devices.
2308.14310v1
2023-08-30
Strengthening from dislocation restructuring and local climb at platelet linear complexions in Al-Cu alloys
Stress-driven segregation at dislocations can lead to structural transitions between different linear complexion states. In this work, we examine how platelet array linear complexions influence dislocation motion and quantify the associated strengthening effect in Al-Cu alloys using atomistic simulations. The presence of platelet complexions leads to faceting of the dislocations, with nanoscale segments climbing upwards along the platelet growth direction, resulting in a complex non-planar configuration that restricts subsequent dislocation motion. Upon deformation, the leading partial dislocation must climb down from the platelet complexions first, followed by a similar sequence at the trailing partial dislocation, in order to overcome the precipitates and commence plastic slip. The dislocation depinning mechanism of linear complexions is strikingly different from traditional precipitation-strengthened alloys, where dislocations overcome obstacles by either shearing through or looping around obstacles. The critical shear stress required to unpin dislocations from platelet complexions is found to be inversely proportional to precipitate spacing, which includes not just the open space (as observed in Orowan bowing) but also the region along the platelet particle where climb occurs. Thus, platelet linear complexions provide a new way to modify dislocation structure directly and improve the mechanical properties of metal alloys.
2308.16117v2
2023-09-23
Enhanced radiation damage tolerance of amorphous interphase and grain boundary complexions in Cu-Ta
Amorphous interfacial complexions are particularly resistant to radiation damage and have been primarily studied in alloys with good glass-forming ability, yet recent reports suggest that these features can form even in immiscible alloys such as Cu-Ta under irradiation. In this study, the mechanisms of damage production and annihilation due to primary knock-on atom collisions are investigated for amorphous interphase and grain boundaries in a Cu-Ta alloy using atomistic simulations. Amorphous complexions, in particular amorphous interphase complexions that separate Cu and Ta grains, result in less residual defect damage than their ordered counterparts. Stemming from the nanophase chemical separation in this alloy, the amorphous complexions exhibit a highly heterogeneous distribution of atomic excess volume, as compared to a good glass former like Cu-Zr. Complexion thickness, a tunable structural descriptor, plays a vital role in damage resistance. Thicker interfacial films are more damage-tolerant because they alter the defect production rate due to differences in intrinsic displacement threshold energies during the collision cascade. Overall, the findings of this work highlight the importance of interfacial engineering in enhancing the properties of materials operating in radiation-prone environments and the promise of amorphous complexions as particularly radiation damage-tolerant microstructural features.
2309.13474v2
2023-10-16
Variations of Interatomic Force Constants in the Topological Phonon Phase Transition of AlGaN
The topological effects of phonons have been extensively studied in various materials, particularly in the wide-bandgap semiconductor GaN, which has the potential to improve heat dissipation in power electronics due to its intrinsic, topologically-protected, non-dissipative phonon surface states. Nevertheless, the phase transition of the Weyl phonons in nitrides and their composite alloys has yet to be elucidated. To unveil the microscale origin, topological phonon properties in AlGaN alloys are investigated using the virtual crystal approximation (VCA) and special quasi-random structure (SQS) approaches in this work. It is found that phase transitions in Weyl phonons are evidently present in AlGaN alloys and nitride single crystals. Under strain states, both GaN and AlN show a more prominent phase transition of Weyl phonons when subjected to biaxial compressive and uniaxial tensile strains. And it has been observed that the zz components in the self-term and the transverse 1NN force constants (FCs) are the most influential during the phase transition. The nonlinear Weyl phonon transition in AlGaN alloys, as modeled by the VCA, is reflected in the normalized self-term and first-nearest-neighbor (1NN) FCs, which vary in a nonlinear fashion with an increasing magnitude. This nonlinear phenomenon is also confirmed in the SQS modeling, where the unfolded phonon dispersions are consistent with those in the VCA modeling. With increased branches, hundreds of Weyl phonons are present accompanied by significant disorders in normalized FCs, which mainly occur for N atoms in self-terms and for all components in normalized 1NN FCs.
2310.09996v1
2023-10-19
Automated Repair of Declarative Software Specifications in the Era of Large Language Models
The growing adoption of declarative software specification languages, coupled with their inherent difficulty in debugging, has underscored the need for effective and automated repair techniques applicable to such languages. Researchers have recently explored various methods to automatically repair declarative software specifications, such as template-based repair, feedback-driven iterative repair, and bounded exhaustive approaches. The latest developments in large language models provide new opportunities for the automatic repair of declarative specifications. In this study, we assess the effectiveness of utilizing OpenAI's ChatGPT to repair software specifications written in the Alloy declarative language. Unlike imperative languages, specifications in Alloy are not executed but rather translated into logical formulas and evaluated using backend constraint solvers to identify specification instances and counterexamples to assertions. Our evaluation focuses on ChatGPT's ability to improve the correctness and completeness of Alloy declarative specifications through automatic repairs. We analyze the results produced by ChatGPT and compare them with those of leading automatic Alloy repair methods. Our study revealed that while ChatGPT falls short in comparison to existing techniques, it was able to successfully repair bugs that no other technique could address. Our analysis also identified errors in ChatGPT's generated repairs, including improper operator usage, type errors, higher-order logic misuse, and relational arity mismatches. Additionally, we observed instances of hallucinations in ChatGPT-generated repairs and inconsistency in its results. Our study provides valuable insights for software practitioners, researchers, and tool builders considering ChatGPT for declarative specification repairs.
2310.12425v2
2023-11-30
Criteria to observe single-shot all-optical switching in Gd-based ferrimagnetic alloys
Single-shot all-optical helicity-independent switching (AO-HIS) induced by a femto-second laser pulse has been mainly reported in Gadolinium based rare earth-transition metal (RE-TM) alloys such as GdFeCo or GdCo, but the mechanism leading to magnetization switching is a hotly debated topic. Here, we elaborate on a large number of GdyRE1-x-yCox (RE = Dy, Tb, Ho) alloys to tune various magnetic parameters in order to define what the criteria are for observing AO-HIS in such systems. The state diagrams show that two laser fluences thresholds must be considered:the fluence which induces the single laser pulse switching (FSwitch) and the fluence at which the material breaks into a multi-domain state (FMulti). Those two fluences are shown to behave very differently as a function of the material properties and the laser pulse duration. Taking into account the parameters defining the conditions for which multi-domain states are created and considering only the angular momentum transfer from the Gd sublattice to the rest of the system explains in large our experimental results. The importance of the compensation in the ferrimagnetic alloys is also discussed. We believe the defined criteria will be an important tool for designing new ultra-fast spintronic devices based on all optical switching.
2311.18359v1
2024-01-01
Tuning Thermal Conductivity of Hybrid Perovskites through Halide Alloying
Tuning the thermal transport properties of hybrid halide perovskites is critical for their applications in optoelectronics, thermoelectrics, and photovoltaics. Here, we demonstrate an effective strategy to modulate the thermal transport property of hybrid perovskites by halide alloying. A highly tunable thermal conductivity of mixed-halide hybrid perovskites is achieved due to halide-alloying and structural distortion. Our experimental measurements show that the room temperature thermal conductivity of MAPb(BrxI1-x)3 (x = 0-1) can be largely modulated from 0.27 W/mK (x = 0.5) to 0.47 W/mK (x = 1). Molecular dynamics simulations further demonstrate that the thermal conductivity reduction of hybrid halide perovskites results from the suppression of the mean free paths of the low-frequency acoustic and optical phonons. It is found that halide alloying and the induced structural distortion can largely increase the scatterings of optical and acoustic phonons, respectively. The confined diffusion of MA+ cations in the octahedra cage is found to act as an additional thermal transport channel in hybrid perovskites and can contribute around 10-20% of the total thermal conductivity. Our findings provide a strategy for tailoring the thermal transport in hybrid halide perovskites which may largely benefit their related applications.
2401.00647v1
2024-02-02
Predictive Models based on Deep Learning Algorithms for Tensile Deformation of AlCoCuCrFeNi High-entropy alloy
High-entropy alloys (HEAs) stand out between multi-component alloys due to their attractive microstructures and mechanical properties. In this investigation, molecular dynamics (MD) simulation and machine learning were used to ascertain the deformation mechanism of AlCoCuCrFeNi HEAs under the influence of temperature, strain rate, and grain sizes. First, the MD simulation shows that the yield stress decreases significantly as the strain and temperature increase. In other cases, changes in strain rate and grain size have less effect on mechanical properties than changes in strain and temperature. The alloys exhibited superplastic behavior under all test conditions. The deformity mechanism discloses that strain and temperature are the main sources of beginning strain, and the shear bands move along the uniaxial tensile axis inside the workpiece. Furthermore, the fast phase shift of inclusion under mild strain indicates the relative instability of the inclusion phase of HCP. Ultimately, the dislocation evolution mechanism shows that the dislocations are transported to free surfaces under increased strain when they nucleate around the grain boundary. Surprisingly, the ML prediction results also confirm the same characteristics as those confirmed from the MD simulation. Hence, the combination of MD and ML reinforces the confidence in the findings of mechanical characteristics of HEA. Consequently, this combination fills the gaps between MD and ML, which can significantly save time human power and cost to conduct real experiments for testing HEA deformation in practice.
2402.01578v1
2024-02-03
Lattice-dynamics and in-plane antiferromagnetism in MnxZn1_xPS3 across the entire composition range
Alloyed MnxZn1_xPS3 samples have been grown covering the whole compositional range and studied by means of Raman spectroscopy at temperatures covering from 4K up to 850K. Our results, supported by SQUID magnetic measurements, allowed, from one hand, to complete the magnetic phase diagram of MnxZn1_xPS3 and establish x>0.3 as the composition at which the alloy retains antiferromagnetism and, from the other hand, to identify the Raman signatures indicative of a magnetic transition. The origin of these Raman signatures is discussed in terms of spin-phonon coupling resulting in the appearance of low- and high-frequency zone-folded phonon modes. For the alloy, an assignment of the 1st and 2nd order modes is provided with the aid of first-principle lattice-dynamical calculations. The compositional dependence of all phonon modes is described and the presence of zone-folded modes is shown to take place for both, the alloy and MnPS3. Finally, a comparison of the Raman spectra of ZnPS3 to other compounds of the transition-metal phosphorous trisulfide family allowed shows that low-frequency phonon peaks exhibit an abnormally large broadening. This is consistent with previous claims on the occurrence of a second-order Jahn-Teller effect that takes place for ZnPS3 and Zn-rich MnxZn1_xPS3.
2402.02102v1
2024-02-04
Origin of the low precipitation hardening in magnesium alloys
In this work electron backscattered diffraction (EBSD)-assisted slip trace analysis and transmission electron microscopy have been utilized to investigate the interaction of basal dislocations with precipitates in the Mg alloys Mg-1%wt.Mn-0.7%wt.Nd (MN11) and Mg-9%wt.Al-1%wt.Zn (AZ91), with the ultimate aim of determining the origin of their poor precipitation hardening. Precipitates in these alloys have a plate-shaped morphology, with plates being, respectively, perpendicular (MgxNdy) and parallel (Mg17Al12) to the basal plane of the magnesium matrix. Mechanical tests were carried out in solid solution and peak-aged samples, in tension and compression, both at RT and at moderate temperature (250C). EBSD-assisted slip trace analysis revealed a clear dominance of basal slip under a wide range of testing conditions in the peak-aged MN11 and AZ91 alloys. At room temperature, the origin of the low precipitation hardening observed lies at the easiness with which precipitates are sheared by basal dislocations, due to the lattice matching at the interface with the Mg matrix. At high temperature, dislocation-precipitate interactions are highly dependent on the deformation mode. In tension, enhanced basal slip localization gives rise to high stress concentrations at the intersection between coarse slip traces and particle interfaces, leading to precipitate fracture; in compression, a more homogenous distribution of basal slip leads to the dominance of particle shearing. Our study demonstrates experimentally that basal dislocations are able to shear, and even fracture, the MgxNdy and Mg17Al12 plates when, for appropriate testing conditions, the local stress due to dislocation accumulation at particle interfaces exceeds the precipitate strength.
2402.06652v1
2024-02-13
Chemical tuning of photo- and persistent luminescence of Cr3+-activated beta-Ga2O3 by alloying with Al2O3 and In2O3
An effect of alloying of the monoclinic beta- Ga2O3 with Al2O3 and In2O3 on the photoluminescent, thermoluminescent and persistent luminescent properties of Cr3+ ions has been comprehensively investigated. For this purpose, various series of Cr3+ and Ca2+ co-doped microcrystalline phosphors were synthesized by the solution combustion method, including pseudobinary compounds like (Ga-Al)2O3 with up to 20% Al and (Ga-In)2O3 with up to 50% In as well as pseudoternary compounds (Ga Al In)2O3 with balanced proportion of Al, Ga and In. The phase composition and crystal structure of the obtained materials were examined by X-ray powder diffraction technique. Detailed luminescence studies were conducted for the (Ga-Al)2O3 and (Ga-In)2O3 compounds which exhibited a single-phase monoclinic structure. Low-temperature and time-resolved photoluminescence investigations of the Cr-doped pseudobinary compounds unveiled several types of Cr3+ centres, attributed to the Al-, Ga- and In-centred octahedra in the studied alloys. The obtained results underscore the benefit of bandgap engineering through alteration in the host lattice chemical composition for efficient tuning of the thermoluminescent and persistent luminescent properties of the near-infrared-emitting beta Ga2O3:Cr based phosphors. Furthermore, it was demonstrated that modification of the chemical composition of the host lattice also adjusts the thermometric performance of the studied phosphors. Indeed, the specific sensitivity of the beta- Ga2O3:Cr3+ decay time luminescence thermometer showed nearly twofold enhancement when the host lattice was alloyed with 30% of In2O3.
2402.08542v2
2024-02-14
Towards a dynamically reconfigurable pixelated reflective display: Focused ion beam for phase-change metapixel structures
The switching and optical properties of phase-change thin films are actively investigated for future smart optical devices. The possibility of having more than one stable state, the large optical contrast between phases, and the fast and reversible switching are some attractive properties driving the research interest. Optical devices based on phase change alloys are considered the frontier contenders for tunable photonics. The combination of vivid structural color formation, with partial amorphization/crystallization of phase change alloys, and the associated optical tunability could be integrated into an energy-efficient reflective display device with high pixel density. This work demonstrates a contrast formation due to relative height differences from isolated pixelated structures. A reflective heterostructure device consisting of a low-loss Sb2Se3 alloy on a gold substrate was produced. With a focused ion beam, a pixelated metasurface structure was produced. Moreover, the ability to create local height differences using an ion beam was employed to create a structural color combination mimicking traditional LED like RGB pixels. We believe our approach in creating metapixels on phase change thin film surfaces could open up research interest in phase change alloys and moving away from semi/static plasmonic systems into truly dynamic display devices.
2402.08891v1
2024-02-19
Data-driven study of composition-dependent phase compatibility in NiTi shape memory alloys
The martensitic transformation in NiTi-based Shape Memory Alloys (SMAs) provides a basis for shape memory effect and superelasticity, thereby enabling applications requiring solid-state actuation and large recoverable shape changes upon mechanical load cycling. In order to tailor the transformation to a particular application, the compositional dependence of properties in NiTi-based SMAs, such as martensitic transformation temperatures and hysteresis, has been exploited. However, the compositional design space is large and complex, and experimental studies are expensive. In this work, we develop an interpretable piecewise linear regression model that predicts the $\lambda_2$ parameter, a measure of compatibility between austenite and martensite phases, and an (indirect) factor that is well-correlated with martensitic transformation hysteresis, based on the chemical features derived from the alloy composition. The model is capable of predicting, for the first time, the type of martensitic transformation for a given alloy chemistry. The proposed model is validated by experimental data from the literature as well as in-house measurements. The results show that the model can effectively distinguish between $B19$ and $B19^{\prime}$ regions for any given composition in NiTi-based SMAs and accurately estimate the $\lambda_2$ parameter. Our analysis also reveals that the weighted average of the quotient of the first ionization energy and the Voronoi coordination number is a key compositional characteristic that correlates with the $\lambda_2$ parameter and thermodynamic responses, including the transformation hysteresis, martensite start temperature, and critical temperature. The work herein demonstrates the potential of data-driven methodologies for understanding and designing NiTi-based SMAs with desired transformation characteristics.
2402.12520v1
2024-03-06
Collision Cascade-Driven Evolution of Vacancy Defects in Ni-Based Concentrated Solid-Solution Alloys
Concentrated solid--solution alloys (CSAs) in single--phase form have recently garnered considerable attention owing to their potential for exceptional irradiation resistance. This computational study delves into the intricate interplay of alloying elements on the generation, recombination, and evolution of irradiation-induced defects. Molecular dynamics simulations were conducted for collision cascades at room temperature, spanning a range of primary knock-on atom energies from 1 to 10 keV. The investigation encompasses a series of model crystals, progressing from pure Ni to binary CSAs such as NiFe$_{20}$, NiFe, NiCr$_{20}$, and culminating in the more intricate NiFeCr$_{20}$ CSA. We observe that materials rich in chromium actively facilitate dislocation emissions and induce the nucleation of stacking fault tetrahedra in the proximity of nanovoids, owing to Shockley partial interactions. This result is validated by molecular static simulations, which calculate the surface, vacancy, and defect formation energies. Among various shapes considered, the spherical void proves to be the most stable, followed by the truncated octahedron and octahedron shapes. On the other hand, the tetrahedron cubic shape is identified as the most unstable, and stacking fault tetrahedra exhibit the highest formation energy. Notably, among the materials studied, NiCr$_{20}$ and NiFeCr$_{20}$ CSAs stood out as the sole alloys capable of manifesting this mechanism, mainly observed at high impact energies.
2403.03922v1
2024-03-14
A general-purpose neural network potential for Ti-Al-Nb alloys towards large-scale molecular dynamics with ab initio accuracy
High Nb-containing TiAl alloys exhibit exceptional high-temperature strength and room-temperature ductility, making them widely used in hot-section components of automotive and aerospace engines. However, the lack of accurate interatomic interaction potentials for large-scale modeling severely hampers a comprehensive understanding of the failure mechanism of Ti-Al-Nb alloys and the development of strategies to enhance the mechanical properties. Here, we develop a general-purpose machine-learned potential (MLP) for the Ti-Al-Nb ternary system by combining the neural evolution potentials framework with an active learning scheme. The developed MLP, trained on extensive first-principles datasets, demonstrates remarkable accuracy in predicting various lattice and defect properties, as well as high-temperature characteristics such as thermal expansion and melting point for TiAl systems. Notably, this potential can effectively describe the key effect of Nb doping on stacking fault energies and formation energies. Of practical importance is that our MLP enables large-scale molecular dynamics simulations involving tens of millions of atoms with ab initio accuracy, achieving an outstanding balance between computational speed and accuracy. These results pave the way for studying micro-mechanical behaviors in TiAl lamellar structures and developing high-performance TiAl alloys towards applications at elevated temperatures.
2403.09529v1
2024-03-22
Single-layer of Bi$_{1-x}$Sb$_x$ grown on Ag(111)
In this work, we report the growth of a single mixed Bi$_{1-x}$Sb$_x$ layer, with diverse stoichiometries, on a Ag(111) substrate. The atomic geometry has been thoroughly investigated by low energy electron diffraction, scanning tunneling microscopy, and X-ray photoelectron spectroscopy experiments, as well as calculations based on density functional theory (DFT). We first determined that both pure systems (Bi/Ag(111) and Sb/Ag(111)) show similar behaviors: they form surface alloys with ($\sqrt{3}\times\sqrt{3}$)R30$^\circ$ periodicity for coverages lower than 1/3 ML, and undergo a dealloying transition for higher coverages up to 2/3 ML. We then established a simple preparation procedure to obtain a mixed Bi-Sb overlayer on Ag(111): it is essential to start with a surface completely covered by either of the two pure surface alloys and then deposit the other element on it. The energetics derived from DFT calculations provide insight into the systems preference towards the formation of this phase, and also predict a pathway to the formation of Bi-rich non-alloyed phases. The obtained mixed Bi-Sb phase has a lateral atomic arrangement very similar to the one in the non-alloyed phase observed for Sb on Ag(111), with Sb and Bi atoms distributed disorderly, and presents a significant vertical corrugation, promising considerable Rashba effects.
2403.15242v1
2024-04-09
A Machine Learning Framework for the Prediction of Grain Boundary Segregation in Chemically Complex Environments
The discovery of complex concentrated alloys has unveiled materials with diverse atomic environments, prompting the exploration of solute segregation beyond dilute alloys. Data-driven methods offer promising for modeling segregation in such chemically complex environments, and are employed in this study to understand segregation behavior of a refractory complex concentrated alloy, NbMoTaW. A flexible methodology is developed that uses composable computational modules, with different arrangements of these modules employed to obtain site availabilities at absolute zero and the corresponding density of states beyond the dilute limit, resulting in an extremely large dataset containing 10 million data points. The artificial neural network developed here can rely solely on descriptions of local atomic environments to predict behavior at the dilute limit with very small errors, while the addition of negative segregation instance classification allows any solute concentration from zero up to the equiatomic concentration for ternary or quaternary alloys to be modeled at room temperature. The machine learning model thus achieves a significant speed advantage over traditional atomistic simulations, being four orders of magnitude faster, while only experiencing a minimal reduction in accuracy. This efficiency presents a powerful tool for rapid microstructural and interfacial design in unseen domains. Scientifically, our approach reveals a transition in the segregation behavior of Mo from unfavorable in simple systems to favorable in complex environments. Additionally, increasing solute concentration was observed to cause anti-segregation sites to begin to fill, challenging conventional understanding and highlighting the complexity of segregation dynamics in chemically complex environments.
2404.06499v1
2024-04-10
The effects of V doping on the intrinsic properties of SmFe10Co2 alloys: a theoretical investigation
The present study focuses on the intrinsic properties of the SmFe10Co2-xVx (x = 0-2) alloys, which includes the SmFe10Co2 alloy, one of the most promising permanent magnets with the ThMn12 type of structure due to its large saturation magnetization (1.78 T), high Curie temperature (Tc = 859 K), and anisotropy field (12 T) experimentally obtained. Unfortunately, its low coercivity (<0.4 T) hinders its use in permanent magnet applications. The effect of V-doping on magnetization, magnetocrystalline anisotropy energy, and Curie temperature is investigated by electronic band structure calculations. The spin-polarized fully relativistic Korringa-Kohn-Rostoker (SPR-KKR) band structure method, which employs the coherent potential approximation (CPA) to deal with substitutional disorder, has been used. The Hubbard-U correction to local spin density approximation (LSDA +U) was used to account for the large correlation effects due to the 4f electronic states of Sm. The computed magnetic moments and magnetocrystalline anisotropy energies were compared with existing experimental data to validate the theoretical approach's reliability. The exchange-coupling parameters from the Heisenberg model were used for obtaining the mean-field estimated Curie temperature. The magnetic anisotropy energy was separated into contributions from transition metals and Sm, and its relationships with the local environment, interatomic distances, and valence electron delocalization were analyzed. The suitability of the hypothetical SmFe10CoV alloy for permanent magnet manufacture was assessed using the calculated anisotropy field, magnetic hardness, and intrinsic magnetic properties.
2404.06897v1
2024-04-15
Deep image learning of quantitative structure-property relationships of cooper alloys via feature augmentation on Geodesic curve in shape space
Understanding how the structure of materials affects their properties is a cornerstone of materials science and engineering. However, traditional methods have struggled to accurately describe the quantitative structure-property relationships for complex structures. In our study, we bridge this gap by leveraging machine learning to analyze images of materials' microstructures, thus offering a novel way to understand and predict the properties of materials based on their microstructures. We introduce a method known as FAGC (Feature Augmentation on Geodesic Curves), specifically demonstrated for Cu-Cr-Zr alloys. This approach utilizes machine learning to examine the shapes within images of the alloys' microstructures and predict their mechanical and electronic properties. This generative FAGC approach can effectively expand the relatively small training datasets due to the limited availability of materials images labeled with quantitative properties. The process begins with extracting features from the images using neural networks. These features are then mapped onto the Pre-shape space to construct the Geodesic curves. Along these curves, new features are generated, effectively increasing the dataset. Moreover, we design a pseudo-labeling mechanism for these newly generated features to further enhance the training dataset. Our FAGC method has shown remarkable results, significantly improving the accuracy of predicting the electronic conductivity and hardness of Cu-Cr-Zr alloys, with R-squared values of 0.978 and 0.998, respectively. These outcomes underscore the potential of FAGC to address the challenge of limited image data in materials science, providing a powerful tool for establishing detailed and quantitative relationships between complex microstructures and material properties.
2404.09515v1
2015-03-01
Anomalous Hall effect and current spin polarization in Co$_2$FeX (X = Al, Ga, In, Si, Ge, and Sn) Heusler compounds: A systematic {\it ab initio} study
In this paper, we perform a systematic {\it ab initio} study of two principal spin-related phenomena, namely, anomalous Hall effect and current spin polarization, in Co$_2$Fe-based Heusler compounds Co$_2$FeX (X = Al, Ga, In, Si, Ge, Sn) within the generalized gradient approximation (GGA). The accurate full-potential linearized augmented plane-wave method is used. We find that the spin-polarization of the longitudinal current ($P^L$) in Co$_2$FeX (X = Al, Ga, In, Al$_{0.5}$Si$_{0.5}$ and Sn) is $\sim$100 \% even though that of the electronic states at the Fermi level ($P^D$) is not. Further, the other compounds also have a high current spin polarization with $P^L > 85$ \%. This indicates that all the Co$_2$FeX compounds considered are promising for spin-transport devices. Interestingly, $P^D$ is negative in Co$_2$FeX (X = Si, Ge and Sn), differing in sign from the $P^L$ as well as that from the transport experiments. Secondly, the calculated anomalous Hall conductivities (AHCs) are moderate, being within 200 S/cm, and agree well with the available experiments on highly L2$_1$ ordered Co$_2$FeSi specimen although they differ significantly from the reported experiments on other compounds where the B2 antisite disorders were present. Surprisingly, the AHC in Co$_2$FeSi decreases and then changes sign when Si is replaced by Ge and finally by Sn. Third, the calculated total magnetic moments agree well with the corresponding experimental ones in all the studied compounds except Co$_2$FeSi where a difference of 0.3 $\mu_B$/f.u. exists. We also perform the GGA plus on-site Coulomb interaction $U$ calculations in the GGA+$U$ scheme. We find that including the $U$ affects the calculated total magnetic moment, spin polarization and AHC significantly, and in most cases, results in a disagreement with the available experimental results.
1503.00204v1
2019-04-08
Two functionals approach in DFT for the prediction of thermoelectric properties of Fe$_{2}$ScX (X = P, As, Sb) full Heusler compounds
In the quest of new thermoelectric (TE) materials with high power factors, full-Heusler compounds having flat band are found to be promising candidates. In this direction, Fe$_{2}$ScX (X=P,As,Sb) compounds are investigated using mBJ for the band gap and SCAN to describe the electronic bands and phonon properties for TE applications. The band gaps obtained from mBJ are 0.81 eV, 0.69 eV and 0.60 eV for Fe$_{2}$ScX compounds, respectively. The phonon dispersion, phonon density of states (DOS) and partial DOS are calculated. The phonon contributions to specific heat are obtained as a function of temperature under harmonic approximation. The electronic band structutre calculated from mBJ and SCAN functionals are qualitatively compared. The TE parameters are calculated for both hole and electron dopings under semiclassical theory. We use simple, but reasonable method to estimate phonon relaxation time ($\tau_{ph}$). Using the specific heat, estimated $\tau_{ph}$ and slopes (phase velocity) of acoustic branches in the linear region, lattice thermal conductivity ($\kappa_{ph}$) at 300 K is calculated for three compounds. The obtained values of $\kappa_{ph}$ with constant $\tau_{ph}$ are 18.2, 13.6 and 10.3 $Wm^{-1}K^{-1}$, respectively. Finally, the temperature dependent figure of merit $ZT$ values are calculated for optimal carrier concentrations in the doping range considered, to evaluate the materials for TE application. The $ZT$ values for n-type Fe$_{2}$ScX, in 900-1200 K, are 0.34-0.43, 0.40-0.48 and 0.45-0.52, respectively. While, the p-type Fe$_{2}$ScX have $ZT$ of 0.25-0.34, 0.20-0.28 and 0.18-0.26, respectively in the same temperature range. The $ZT$ values suggest that, Fe$_{2}$ScX compounds can be promising materials in high temperature power generation application on successful synthesis and further $\kappa_{ph}$ reduction by methods like nanostructuring.
1904.04322v1
2019-10-11
Band structure tuning of Heusler compounds revisited: Spin- and momentum-resolved electronic structure analysis of compounds with different band filling
Spin-filtered time-of-flight photoelectron momentum microscopy reveals a systematic variation of the band structure within a series of highly spin-polarized ferromagnetic Heusler compounds with increasing number of valence electrons (Co2MnGa, Co2MnSi and Co2Fe0.4Mn0.6Si). The positions of the Fermi energy for minority and majority electrons deviate strongly from a simple band-filling model. Photoexcitation at h$\nu$=6.05 eV (4th harmonic of a Ti:sapphire laser) gives access to the spin-polarization texture P(EB,kx,ky) of the bulk bands in a (kx,ky)-range with diameter 1.4{\AA}$^{-1}$ and energies from the Fermi energy EF to a binding energy of EB=2 eV. The minority bands of Co2MnGa cross the Fermi level, inhibiting half-metallicity; the crossing points allow a precise adjustment of experimental and theoretical majority and minority bands, requiring shifts in opposite directions. The top of the minority band lies only 0.15 eV above EF, i.e. Co2MnGa is much closer to being half-metallic than predicted by calculations. For half-metallic Co2MnSi and Co2Fe0.4Mn0.6Si clear minority band gaps are visible, the topmost occupied minority bands lie 0.5 and 0.35 eV below EF, in reasonable agreement with theory; the exchange splitting is significantly smaller than in theory. The comparison of all three compounds uncovers the surprising fact that with increasing number of valence electrons the frontier majority bands (close to EF) exhibit an increasing deficiency in filling, in comparison with the prediction of a DFT calculation. The same trend is visible in comparison with a DMFT calculation. For s-polarized excitation both half-metallic compounds exhibit nearly complete positive spin polarization close to EF, consistent with previous work in literature.
1910.05205v1
2020-08-26
First-principles electronic structure, phonon properties, lattice thermal conductivity and prediction of figure of merit of FeVSb half-Heusler
In this work, we have studied the electronic structure of a promising thermoelectric half-Heusler FeVSb using FP-LAPW method and SCAN meta-GGA including spin-orbit coupling. Using the obtained electronic structure and transport calculations we try to address the experimental Seebeck coefficient $S$ of FeVSb samples. The good agreement between the experimental and calculated $S$ suggests the band gap could be $\sim$0.7 eV. This is supported by the obtained mBJ band gap of $\sim$0.7 eV. Further, we study and report the phonon dispersion, density of states and thermodynamic properties. The effect of long range Coulomb interactions on phonon frequencies are also included by non-analytical term correction. Under quasi-harmonic approximation, the thermal expansion behaviour upto 1200 K is calculated. Using the first-principles anharmonic phonon calculations, the lattice thermal conductivity $\kappa_{ph}$ of FeVSb is obtained under single-mode relaxation time approximation considering the phonon-phonon interaction. At 300 K, the calculated $\kappa_{ph}$ is $\sim$18.6 W$m^{-1}K^{-1}$ which is higher compared to experimental value. But, above 500 K the calculated $\kappa_{ph}$ is in good agreement with experiment. A prediction of figure of merit $ZT$ and efficiency for p-type and n-type FeVSb is made by finding out optimal carrier concentration. At 1200 K, a maximum $ZT$ of $\sim$0.66 and $\sim$0.44 is expected for p-type and n-type FeVSb, respectively. For p-type and n-type materials, maximum efficiency of $\sim$12.2 \% and $\sim$6.0 \% are estimated for hot and cold temperature of 1200 K and 300 K, respectively. A possibility of achieving n-type and p-type FeVSb by various elemental doping/vacancy is also discussed. Our study is expected to help in further exploring the thermoelectric material FeVSb.
2008.11693v1
2020-12-23
Identifying the fingerprints of topological states by tuning magnetoresistance in a semimetal: the case of topological half-Heusler Pt1-xAuxLuSb
Topological materials often exhibit remarkably linear, non-saturating magnetoresistance (LMR), which is both of scientific and technological importance. However, the role of topologically non-trivial states in the emergence of such a behaviour has eluded clear demonstration in experiments. Here, by reducing the coupling between the topological surface states (TSS) and the bulk carriers we controllably tune the LMR behavior in Pt1-xAuxLuSb into distinct plateaus in Hall resistance, which we show arise from a quantum Hall phase. This allowed us to reveal how smearing of the Landau levels, which otherwise give rise to a quantum Hall phase, results in an LMR behavior due to strong interaction between the TSS with a positive g-factor and the bulk carriers. We establish that controlling the coupling strength between the surface and the bulk carriers in topological materials can bring about dramatic changes in their magnetotransport behavior. In addition, our work outlines a strategy to reveal macroscopic physical observables of TSS in compounds with a semi-metallic bulk band structure, as is the case in multi-functional Heusler compounds, thereby opening up opportunities for their utilization in hybrid quantum structures.
2012.12633v5
2021-01-23
Studying the lifetime of charge and heat carriers due to intrinsic scattering mechanisms in FeVSb half-Heusler thermoelectric
This work, presents a study of lifetime of carriers due to intrinsic scattering mechanisms $viz.$ electron-electron (EEI), electron-phonon (EPI) and phonon-phonon interactions (PPI) in a promising half-Heusler thermoelectric FeVSb. Using the full-$GW$ method, the effect of EEI and temperature on the valence and conduction band extrema and band gap are studied. The lifetime of carriers with temperature are estimated at these band extrema. At 300 K, estimated value of lifetime at VBM (CBM) is $\sim$1.91 x10$^{-14}s$ ($\sim$2.05 x10$^{-14}s$). The estimated ground state band gap considering EEI is $\sim$378 meV. Next, the effect of EPI on the lifetime of electrons and phonons with temperature are discussed. The comparison of two electron lifetimes suggests that EEI should be considered in transport calculations along with EPI. The average acoustic, optical and overall phonon lifetimes due to EPI are studied with temperature. Further, the effect of PPI is studied by computing average phonon lifetime for acoustic and optical phonon branches. The lifetime of the acoustic phonons are higher compared to optical phonons which indicates acoustic phonons contribute more to lattice thermal conductivity ($\kappa_{ph}$). The comparison of phonon lifetime due to EPI and PPI suggests that, above 500 K EPI is the dominant phonon scattering mechanism and cannot be ignored in $\kappa_{ph}$ calculations. Lastly, a prediction of the power factor and figure of merit of n-type and p-type FeVSb is made by considering the temperature dependent carrier lifetime for the electronic transport terms. This study shows the importance of considering EEI in electronic transport calculations and EPI in phonon transport calculations. Our study is expected to provide results to further explore the thermoelectric transport in this material.
2101.09555v1
2022-06-22
Non-trivial topological phases in transition metal rich half-Heusler Oxides
Topological Insulators with gapless surface states and insulating bulk in non-centrosymmetric cubic systems have been extensively explored following the discovery of two-dimensional quantum spin hall effect in zincblende HgTe. In such systems the negative band inversion strength E$_{BIS}$ ($=$ E$_{\Gamma_6} -$ E$_{\Gamma_8} <$ 0) governs the robustness of the non-trivial topological states at ambient conditions. Hence, realizing large negative values of E$_{BIS}$ has been a guiding motivation of several investigations reported in literature. Here, we present a material design approach which can be employed to realize large negative values of E$_{BIS}$ in cubic materials such as half-Heusler (HH) oxides with 18 valence electron configurations. We explore 27 HH oxides of the form ABO (A = Li, K, Rb; B = Cu, Ag, Au) in $\alpha$-, $\beta$-, and $\gamma$-phase (by placing transition metal atom at different Wyckoff positions) for their non-trivial topological phase. Off these three phases, we found that, the $\alpha$-phase of nine HH oxides (wherein the transition metal atoms occupy 4a Wyckoff positions in the crystal structure) is the most promising with non-trivial topological phase which is governed by the mass-darwin relativistic effects enhancing E$_{BIS}$. Whereas the other phases were found to be either trivial semiconductors or semimetals or metals and most of them being dynamically unstable. We focus on RbAuO in $\alpha$-phase with E$_{BIS}$ of $-$ 1.29 eV and the effect of strain fields on the topological surface states of this compound. We conclude that the $\alpha$-phase of HH oxide presented here can be synthesized experimentally for diverse room temperature applications in spintronics and nanoelectronics.
2206.10976v2
1995-08-17
Weighted two particle Green's functions in the CPA
We extend the two particle theory of disordered systems within the coherent potential approximation CPA to obtain weighted contributions to averaged two particle resolvents which arise from separate alloy components. Starting from first principles in a model of diagonal disorder and the single site approximation for a binary substitutional alloy $A_cB_{1-c}$ we extend the approach of a fundamental paper by Velick{\'y} to evaluate various weighted forms of a general class of two particle Green's functions. Applications in a wide range of linear response theory are discussed in detail as well as the behavior of the weighted functions in a strong disorder limit. To exemplify our analytic calculations the optical absorption in a disordered model- alloy is studied numerically.
9508068v1
1996-04-24
Monte Carlo study of the growth of $L1_2$ ordered domains in fcc $A_3B$ binary alloys
A Monte Carlo study of the late time growth of $L1_2$ ordered domains on a fcc $A_3B$ binary alloy is presented. The energy of the alloy has been modeled by a nearest neighbor interaction Ising hamiltonian. The system exhibits a fourfold degenerated ground-state and two kinds of interfaces separating ordered domains: flat and curved antiphase boundaries. Two different dynamics are used in the simulations: the standard atom-atom exchange mechanism and the more realistic vacancy-atom exchange mechanism. The results obtained by both methods are compared. In particular we study the time evolution of the excess energy, the structure factor and the mean distance between walls. In the case of atom-atom exchange mechanism anisotropic growth has been found: two characteristic lengths are needed in order to describe the evolution. Contrarily, with the vacancy-atom exchange mechanism scaling with a single length holds. Results are contrasted with existing experiments in $Cu_3Au$ and theories for anisotropic growth.
9604150v1
1996-09-19
Disorder-driven non-Fermi liquid behavior in Kondo alloys
We demonstrate that a model of disordered Anderson lattices can account for many non-Fermi liquid features observed in a number of Kondo alloys. Due to the exponential nature of the Kondo temperature scale, even moderate disorder leads to a rather broad distribution of Kondo temperatures, inducing strong effective disorder seen by the conduction electrons. Spins with very small Kondo temperatures remain unquenched and dominate the low temperature properties. The model predicts logarithmic divergences in thermodynamic quantities at low temperatures. We also find a linear temperature dependence of the resistivity, a feature that remained a stumbling block in previous theoretical attempts. We argue that for realistic amounts of disorder, such marginal Fermi liquid behavior is a very robust feature of disordered Kondo alloys.
9609193v1
1996-09-20
Electronic structure of the valence band of the II--VI wide band gap binary/ternary alloy interfaces
We present an electronic structure calculation of the valence band for some II--VI binary/ternary alloy interfaces. We use the empirical tight-binding method and the surface Green's function matching method. For the ternary alloys we use our previously set Hamiltonians they describe well the band gap change with composition obtained experimentally. At the interface domain, we find three non-dispersive and two interface states besides the known bulk bands. The non-dispersive states are reminiscent of the ones already obtained experimentally as well as theoretically, in (001)-oriented surfaces. We make use of the available theoretical calculations for the (001)-oriented surfaces of the binary compounds and for the binary/binary interfaces to compare our new results with.
9609196v1
1996-11-28
Thermal and Mechanical Properties of Pt-Rh Alloys
We utilize the many-body potentials developed by Sutton and Chen(1990) within the context of the tight-binding approach to study the bulk properties of metals and metal alloys in molecular dynamics (MD) simulations. In the simulations of Pt-Rh alloys we used the MD algorithms based on an extended Hamiltonian formalism from the works of Andersen(1980), Parrinello and Rahman(1980), Nose(1984), Hoover(1985) and Cagin(1988).The simulator program that we use generates information about various physical properties during the run time, along with critical trajectory and stepwise information which need to be analysed post production. The thermodynamical and mechanical properties are calculated using the statistical fluctuation expressions over the MD.
9611241v1
1998-08-05
Theoretical search for Chevrel phase based thermoelectric materials
We investigate the thermoelectric properties of some semiconducting Chevrel phases. Band structure calculations are used to compute thermopowers and to estimate of the effects of alloying and disorder on carrier mobility. Alloying on the Mo site with transition metals like Re, Ru or Tc to reach a semiconducting composition causes large changes in the electronic structure at the Fermi level. Such alloys are expected to have low carrier mobilities. Filling with transition metals was also found to be incompatible with high thermoelectric performance based on the calculated electronic structures. Filling with Zn, Cu, and especially with Li was found to be favorable. The calculated electronic structures of these filled Chevrel phases are consistent with low scattering of carriers by defects associated with the filling. We expect good mobility and high thermopower in materials with the composition close to (Li,Cu)$_4$Mo$_6$Se$_8$, particularly when Li-rich, and recommend this system for experimental investigation.
9808056v1
1999-03-07
Correlation between Spin Polarization and Magnetic Moment in Ferromagnetic Alloys
The correlation between the magnetic moment in ferromagnetic alloys and the tunneling spin polarization in ferromagnet-insulator-superconductor tunneling experiments has been a mystery. The measured spin polarization for Fe, Co, Ni, and various Ni alloys is positive and roughly proportional to their magnetic moments, which can not be explained by considering the net density of states. Using a tight-binding coherent potential approximation (CPA) model, we show that while the polarization of the net density of states is not correlated with the magnetic moment, the polarization of the density of states of {\it s} electrons is correlated with the magnetic moment in the same manner as observed by the tunneling experiments. We also discuss the spin polarization measurements by Andreev reflection experiments, some of which obtained different results from the tunneling experiments and our calculations.
9903118v2
1999-10-26
Depletion of density of states near Fermi energy induced by disorder and electron correlation in alloys
We have performed high resolution photoemission study of substitutionally disordered alloys Cu-Pt, Cu-Pd, Cu-Ni, and Pd-Pt. The ratios between alloy spectra and pure metal spectra are found to have dips at the Fermi level when the residual resistivity is high and when rather strong repulsive electron-electron interaction is expected. This is in accordance with Altshuler and Aronov's model which predicts depletion of density of states at the Fermi level when both disorder and electron correlation are present.
9910411v1
2000-08-02
Superconducing Alloys with Weak and Strong Scattering: Anderson's Theorem and a Superconductor-Insulator Transition
We have studied the effects of strong impurity scattering on disordered superconductors beyond the low impurity concentration limit. By applying the full CPA to a superconductiong A-B binary alloy, we calculated the fluctuations of the local order parameters $\Delta_{A}, \Delta_{B}$ and charge densities, $n_{A}, n_{B}$ for weak and strong on site disorder. We find that for narrow band alloy s-wav e superconductors the conditions for Anderson's theorem are satisfied in general only for the case of particle-hole symmetry. In this case it is satisfied regardless whether we are in the weak or strong scattering regimes. Interestingly, we find that strong scattering leads to band splitting and in this regime for any band filling we have a critical concentration where a superconductor-insulator quantum phase transition occurs at T=0.
0008031v1
2000-08-04
Local structure study of In_xGa_(1-x)As semiconductor alloys using High Energy Synchrotron X-ray Diffraction
Nearest and higher neighbor distances as well as bond length distributions (static and thermal) of the In_xGa_(1-x)As (0<x<1) semiconductor alloys have been obtained from high real-space resolution atomic pair distribution functions (PDFs). Using this structural information, we modeled the local atomic displacements in In_xGa_(1-x)As alloys. From a supercell model based on the Kirkwood potential, we obtained 3-D As and (In,Ga) ensemble averaged probability distributions. This clearly shows that As atom displacements are highly directional and can be represented as a combination of <100> and <111> displacements. Examination of the Kirkwood model indicates that the standard deviation (sigma) of the static disorder on the (In,Ga) sublattice is around 60% of the value on the As sublattice and the (In,Ga) atomic displacements are much more isotropic than those on the As sublattice. The single crystal diffuse scattering calculated from the Kirkwood model shows that atomic displacements are most strongly correlated along <110> directions.
0008079v1
2000-08-30
Ferromagnetism in the Periodic Anderson Model - a Modified Alloy Analogy
We introduce a new aproximation scheme for the periodic Anderson model (PAM). The modified alloy approximation represents an optimum alloy approximation for the strong coupling limit, which can be solved within the CPA-formalism. Zero-temperature and finite-temperature phase diagrams are presented for the PAM in the intermediate-valence regime. The diversity of magnetic properties accessible by variation of the system parameters can be studied by means of quasiparticle densities of states: The conduction band couples either ferro- or antiferromagneticaly to the f-levels. A finite hybridization is a necessary precondition for ferromagnetism. However, too strong hybridization generally suppresses ferromagnetism, but can for certain system parameters also lead to a semi-metallic state with unusual magnetic properties. By comparing with the spectral density approximation, the influence of quasiparticle damping can be examined.
0008441v1
2000-11-03
Charge transfer electrostatic model of compositional order in perovskite alloys
We introduce an electrostatic model including charge transfer, which is shown to account for the observed B-site ordering in Pb-based perovskite alloys. The model allows charge transfer between A-sites and is a generalization of Bellaiche and Vanderbilt's purely electrostatic model. The large covalency of Pb^{2+} compared to Ba^{2+} is modeled by an environment dependent effective A-site charge. Monte Carlo simulations of this model successfully reproduce the long range compositional order of both Pb-based and Ba-based complex A(BB^{'}B^{''})O_3 perovskite alloys. The models are also extended to study systems with A-site and B-site doping, such as (Na_{1/2}La_{1/2})(Mg_{1/3}Nb_{2/3})O_3, (Ba_{1-x}La_{x})(Mg_{(1+x)/3}Nb_{(2-x)/3})O_3 and (Pb_{1-x}La_{x})(Mg_{(1+x)/3}Ta_{(2-x)/3})O_3. General trends are reproduced by purely electrostatic interactions, and charge transfer effects indicate that local structural relaxations can tip the balance between different B-site orderings in Pb based materials.
0011063v1
2000-12-13
Strain Relaxation Mechanisms and Local Structural Changes in Si_{1-x}$Ge_{x} Alloys
In this work, we address issues pertinent to the understanding of the structural and electronic properties of Si_{1-x} Ge_{x}alloys, namely, (i) how does the lattice constant mismatch between bulk Si and bulk Ge manifests itself in the alloy system? and (ii) what are the relevant strain release mechanisms? To provide answers to these questions, we have carried out an in-depth study of the changes in the local geometric and electronic structures arising from the strain relaxation in Si_{1-x} Ge_{x} alloys using an ab initio molecular dynamics scheme. The optimized lattice constant, while exhibiting a general trend of linear dependence on the composition (Vegard's law), shows a negative deviation from Vegard's law in the vicinity of x=0.5. We delineate the mechanisms responsible for each one of the above features. We show that the radial-strain relaxation through bond stretching is responsible for the overall trend of linear dependence of the lattice constant on the composition. On the other hand, the negative deviation from Vegard's law is shown to arise from the angular-strain relaxation.
0012220v1
2001-08-09
Elastic and thermodynamic properties of the shape-memory alloy AuZn
The current work reports on the elastic shear moduli, internal friction, and the specific heat of the B2 cubic ordered alloy AuZn as a function of temperature. Measurements were made on single-crystal and polycrystalline samples using Resonant Ultrasound Spectroscopy (RUS), semi-adiabatic calorimetry and stress-strain measurements. Our results confirm that this alloy exhibits the shape-memory effect and a phase transition at 64.75 K that appears to be continuous (second-order) from the specific heat data. It is argued that the combination of equiatomic composition and a low transformation temperature constrain the chemical potential and its derivatives to exhibit behavior that lies at the borderline between that of a first-order (discontinuous) and a continuous phase transition. The acoustic dissipation does not peak at the transtion temperature as expected, but shows a maximum well into the low-temperature phase. The Debye temeprature value of 219 K, obtained from the low-temperature specific heat data is in favorable agreement with that determined from the acoustic data (207 K) above the transition.
0108168v1
2001-08-27
Master equation approach to configurational kinetics of non-equilibrium alloys and its application to studies of L1_0 type orderings
We review a series of works where the fundamental master equation is used to develop a microscopical description of evolution of non-equilibrium atomic distributions in alloys. We describe exact equations for temporal evolution of local concentrations and their correlators as well as approximate methods to treat these equations, such as the kinetic mean-field and the kinetic cluster methods. We also describe an application of these methods to studies of kinetics of L1_0 type orderings in FCC alloys which reveal a number of peculiar microstructural effects, many of them agreeing well with experimental observations.
0108441v1
2001-10-27
Dynamics of a single electron in the disordered Holstein model
We study, at zero temperature, the dynamics of a single electron in a Holstein model augmented by site-diagonal, binary-alloy type disorder. The average over the phonon vacuum and the alloy configurations is performed within a generalized dynamical coherent potential approximation. We present numerical results for a Bethe lattice with infinite coordination number. In particular, we investigate, in the intermediate electron-phonon coupling regime, the spectral and diffusion properties in the vicinity of the high-energy edge of the lowest polaronic subband. To characterize the diffusion properties, we define a spectrally resolved delocalization time, which is, for a given energy, the characteristic time scale on which the electron leaves a given site. We find the delocalization times substantially enhanced for states with a large phonon content, i.e., in the absence (presence) of alloy-type disorder at the high-energy edge(s) of the polaronic subband (mini-subbands). According to their delocalization times, we discriminate between ``fast'' quasi-particle-like and ``sluggish'' defect-like polaron states and qualitatively address the issue of trapping of an electronic carrier.
0110577v1
2001-11-01
Metal-insulator transition in amorphous alloys
We focus on the central problem of discriminating between metallic and insulating behaviour in amorphous alloys formed between a semiconductor and a metal. For this, the logarithmic temperature derivative of the conductivity, w = d ln sigma / d ln T, has proved over recent years to be very helpful in determining the critical value x_c of the metal content x for the metal-insulator transition (MIT). We show that, for various amorphous alloys, recent experimental results on w(T,x) are qualitatively inconsistent with the usual assumptions of continuity of the MIT at T = 0 and of sigma(T,x_c) being proportional to a power of T. These results suggest that w(T,x_c) tends to 0 as T -> 0, in which case the MIT should be discontinuous at T = 0 (but only there), in agreement with Mott's hypothesis of a finite minimum metallic conductivity.
0111017v1