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At least 829 records · Page 46
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Neural network-based order parameter for phase transitions and its applications in high-entropy alloys

Phase transition is one of the most important phenomena in nature and plays a central role in materials design. All phase transitions are characterized by suitable order parameters, including the order–disorder phase transition. However, finding a representative order parameter for complex systems is non-trivial, such as for high-entropy alloys. Given the strength of dimensionality reduction of a variational autoencoder (VAE), we introduce a VAE-based order parameter. Here, we propose that the Manhattan distance in the VAE latent space can serve as a generic order parameter for order–disorder phase transitions. The physical properties of our order parameter are quantitatively interpreted and demonstrated by multiple refractory high-entropy alloys. Using this order parameter, a generally applicable alloy design concept is proposed by mimicking the natural mixing process of elements. Our physically interpretable VAE-based order parameter provides a computational technique for understanding chemical ordering in alloys, which can facilitate the development of rational alloy design strategies.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Perfect short-range ordered alloy with line-compound-like properties in the ZnSnN 2 :ZnO system

We present a new solid-state material phase which is a disordered solid solution but offers many ordered line-compound features. The emergent physical phenomena are rooted in the perfect short-range order which conserves the local octet rule. We model the dual-sublattice-mixed semiconductor alloy (ZnSnN 2 ) 1-x (ZnO) 2x using first-principles calculations, Monte-Carlo simulations with a model Hamiltonian, and an extension of the regular solution model by incorporating short-range order. We demonstrate that this unique solid solution, occurring at a “magic” composition, can provide an electronically pristine character without disorder-induced charge localization and, therefore, a superior carrier transport similar to ordered phases. Interestingly, this phase shows singularities that are absent in the conventional solid-solution models, such as the regular solution and band-gap bowing model. Thermodynamically, this alloy phase has a sharply reduced enthalpy at its composition (like a line compound), but it still requires the entropy from long-range disorder to be stabilized at experimentally accessible temperatures.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Thermodynamic non-ideality and disorder heterogeneity in actinide silicate solid solutions

Non-ideal thermodynamics of solid solutions can greatly impact materials degradation behavior. We have investigated an actinide silicate solid solution system (USiO 4 –ThSiO 4 ), demonstrating that thermodynamic non-ideality follows a distinctive, atomic-scale disordering process, which is usually considered as a random distribution. Neutron total scattering implemented by pair distribution function analysis confirmed a random distribution model for U and Th in first three coordination shells; however, a machine-learning algorithm suggested heterogeneous U and Th clusters at nanoscale (~2 nm). The local disorder and nanosized heterogeneous is an example of the non-ideality of mixing that has an electronic origin. Partial covalency from the U/Th 5f–O 2p hybridization promotes electron transfer during mixing and leads to local polyhedral distortions. The electronic origin accounts for the strong non-ideality in thermodynamic parameters that extends the stability field of the actinide silicates in nature and under typical nuclear waste repository conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Attractive Hubbard model with disorder and the generalized Anderson theorem

Using the generalized DMFT+Σ approach, we study the influence of disorder on single-particle properties of the normal phase and the superconducting transition temperature in the attractive Hubbard model. A wide range of attractive potentials U is studied, from the weak coupling region, where both the instability of the normal phase and superconductivity are well described by the BCS model, to the strong-coupling region, where the superconducting transition is due to Bose-Einstein condensation (BEC) of compact Cooper pairs, formed at temperatures much higher than the superconducting transition temperature. We study two typical models of the conduction band with semi-elliptic and flat densities of states, respectively appropriate for three-dimensional and two-dimensional systems. For the semi-elliptic density of states, the disorder influence on all single-particle properties (e.g., density of states) is universal for an arbitrary strength of electronic correlations and disorder and is due to only the general disorder widening of the conduction band. In the case of a flat density of states, universality is absent in the general case, but still the disorder influence is mainly due to band widening, and the universal behavior is restored for large enough disorder. Using the combination of DMFT+Σ and Nozieres-Schmitt-Rink approximations, we study the disorder influence on the superconducting transition temperature T{sub c} for a range of characteristic values of U and disorder, including the BCS-BEC crossover region and the limit of strong-coupling. Disorder can either suppress T{sub c} (in the weak-coupling region) or significantly increase T{sub c} (in the strong-coupling region). However, in all cases, the generalized Anderson theorem is valid and all changes of the superconducting critical temperature are essentially due to only the general disorder widening of the conduction band.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Correlation between Cr 3+ Luminescence and Oxygen Vacancy Disorder in Strontium Titanate under MeV Ion Irradiation

Strontium titanate (SrTiO 3 ), a model system with a strongly correlated electronic structure, has attracted much attention recently because of its outstanding physicochemical properties and considerable potentials for technological applications. The capability to control oxygen vacancy profiles and their effect on valence states of cations will increase significantly the functionality of devices based on transition metal oxides. This work presents new insights into the near-infrared luminescence emission of Cr 3+ centers in stoichiometric SrTiO 3 induced using 3 MeV protons at temperatures of 100 K, 170 K, and room temperature. The study covers a wide spectral range, including near-infrared, visible, and near-UV regions. Our main purpose is to investigate the role of the oxygen vacancies introduced by energetic charged particles on the shape and yield of induced luminescence spectra, in particular to explore the interplay between the Cr 3+ luminescence at 1.55 eV and oxygen disorder. A clear correlation is found between the decay of the Cr luminescence yield during irradiation and the growth of a band at 2.0 eV, well-resolved below 170 K, which has been very recently attributed to d–d transitions of electrons self-trapped as Ti 3+ in the close vicinity of oxygen vacancies. This correlation suggests irradiation-induced oxidation of the Cr 3+ (Cr 3+ → Cr n+ , n > 3) via trapping of irradiation-induced holes, while the partner electrons are self-trapped as Ti 3+ . Here, these new results provide effective guidelines for further understanding the electronic and photocatalytic behavior of STO:Cr 3+ .

36 MATERIALS SCIENCE↗
DOE OSTI2022

Interplay between disorder and collective coherent response: Superradiance and spectral motional narrowing in the time domain

The interplay between static and dynamic disorder and collective optical response in molecular ensembles is an important characteristic of nanoplasmonic and nanophotonic molecular systems. Here we investigate the cooperative superradiant response of a molecular ensemble of quantum emitters under the influence of environmental disorder, including inhomogeneous broadening (as induced by a static random distribution of the molecular transition frequencies) and motional narrowing (as induced by stochastic modulation of these excitation energies). The effect of inhomogeneous broadening is to destroy the coherence of the collective molecular excitation and suppress superradiant emission. However, fast stochastic modulation of the molecular excitation energy can effectively restore the coherence of the quantum emitters and lead to a recovery of superradiant emission, which is an unexpected manifestation of motional narrowing. For a light-scattering process as induced by an off-resonant incident pulse, stochastic modulation leads to inelastic fluorescence emission at the average excitation energy at long times and suggests that dynamic disorder effects can actually lead to collective excitation of the molecular ensemble.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2016

Effects of configurational disorder on the elastic properties of icosahedral boron-rich alloys based on B{sub 6}O, B{sub 13}C{sub 2}, and B{sub 4}C, and their mixing thermodynamics

The elastic properties of alloys between boron suboxide (B{sub 6}O) and boron carbide (B{sub 13}C{sub 2}), denoted by (B{sub 6}O){sub 1−x}(B{sub 13}C{sub 2}){sub x}, as well as boron carbide with variable carbon content, ranging from B{sub 13}C{sub 2} to B{sub 4}C are calculated from first-principles. Furthermore, the mixing thermodynamics of (B{sub 6}O){sub 1−x}(B{sub 13}C{sub 2}){sub x} is studied. A superatom-special quasirandom structure approach is used for modeling different atomic configurations, in which effects of configurational disorder between the carbide and suboxide structural units, as well as between boron and carbon atoms within the units, are taken into account. Elastic properties calculations demonstrate that configurational disorder in B{sub 13}C{sub 2}, where a part of the C atoms in the CBC chains substitute for B atoms in the B{sub 12} icosahedra, drastically increase the Young’s and shear modulus, as compared to an atomically ordered state, B{sub 12}(CBC). These calculated elastic moduli of the disordered state are in excellent agreement with experiments. Configurational disorder between boron and carbon can also explain the experimentally observed almost constant elastic moduli of boron carbide as the carbon content is changed from B{sub 4}C to B{sub 13}C{sub 2}. The elastic moduli of the (B{sub 6}O){sub 1−x}(B{sub 13}C{sub 2}){sub x} system are also practically unchanged with composition if boron-carbon disorder is taken into account. By investigating the mixing thermodynamics of the alloys, in which the Gibbs free energy is determined within the mean-field approximation for the configurational entropy, we outline the pseudo-binary phase diagram of (B{sub 6}O){sub 1−x}(B{sub 13}C{sub 2}){sub x}. The phase diagram reveals the existence of a miscibility gap at all temperatures up to the melting point. Also, the coexistence of B{sub 6}O-rich as well as ordered or disordered B{sub 13}C{sub 2}-rich domains in the material prepared through equilibrium routes is predicted.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Order-disorder behavior at thin film oxide interfaces

Order-disorder processes fundamentally determine the structure and properties of many important oxide systems for energy and computing applications. While these processes have been intensively studied in bulk materials, they are less investigated and understood for nanostructured oxides in highly non-equilibrium conditions. These systems can now be realized through a range of deposition techniques and probed at exceptional spatial and chemical resolution, leading to a greater focus on interface dynamics. In this work, we survey a selection of recent studies of order-disorder behavior at thin film oxide interfaces, with a particular emphasis on the emergence of order during synthesis and disorder in extreme irradiation environments. We summarize key trends and identify directions for future study in this growing research area.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Precisely predicting and designing the elasticity of metallic glasses

We reveal that the elastic moduli of metallic glasses (MGs) invariably vary in a much steeper manner than that predicted by the conventional “rule of mixtures” in individual alloy systems. Such deviations are proved to originate fundamentally from their disordered atomic structures and intrinsic local heterogeneities. By treating the MGs as atomic-level dual phase hybrids, we further propose universal relations to be capable of precisely predicting and designing the elastic constants of MGs. This may contribute to the development of MGs with intended properties and behaviors, and allow new understandings on the structures and properties as well as their relationships in MGs.

42 ENGINEERING↗
DOE OSTI2019

Robustness of entropy plateaus: A case study of triangular Ising antiferromagnets

We present that residual entropy is a key feature associated with emergence in many-body systems. From a variety of frustrated magnets to the onset of spin-charge separation in Hubbard models and fermion-Z 2 -flux variables in Kitaev models, the freezing of one set of degrees of freedom and the establishment of local constraints are marked by a plateau in entropy as a function of temperature. Yet, with the exception of the rare-earth pyrochlore family of spin-ice materials, evidence for such plateaus is rarely seen in real materials, raising questions about their robustness. Following recent experimental findings of the absence of such plateaus in the triangular-lattice Ising antiferromagnet (TIAF) TmMgGaO 4 by Li et al., we explore in detail the existence and rounding of entropy plateaus in TIAF. We use a transfer-matrix method to numerically calculate the properties of the system at different temperatures and magnetic fields, with further neighbor interactions and disorder. In conclusion, we find that temperature windows of entropy plateaus exist only when second-neighbor interactions are no more than a couple of percent of the nearest-neighbor ones, and they are also easily destroyed by disorder in the nearest-neighbor exchange variable, thereby explaining the challenge in observing such effects.

2-dimensional systems↗
DOE OSTI2019

Composition Dependence of the Flory–Huggins Interaction Parameters of Block Copolymer Electrolytes and the Isotaksis Point

The thermodynamics of block copolymer/salt mixtures were quantified through the application of Leibler’s random phase approximation to disordered small-angle X-ray scattering profiles. The experimental system is comprised of polystyrene-block-poly(ethylene oxide) (SEO) mixed with lithium bis(trifluoromethanesulfonyl)imide salt (LiTFSI), SEO/LiTFSI. The Flory–Huggins interaction parameter determined from scattering experiments, χ SC , was found to be a function of block copolymer composition, chain length, and temperature for both salt-free and salty systems. In the absence of salt, χ 0,SC is a linear function of (N$f_{EO}$) -1 ; in the presence of salt, a linear approximation is used to describe the effect of salt on χ eff,SC for a given copolymer composition and chain length. The theory of Sanchez was used to determine χ eff from χ eff,SC to predict the boundary between order and disorder as a function of chain length, block copolymer composition, salt concentration, and temperature. At fixed temperature (100 °C), N crit , the chain length of SEO at the order–disorder transition in SEO/LiTFSI mixtures, was predicted as a function of the volume fraction of the salt-containing poly(ethylene oxide)-rich microphase, $f_{EO,salt,}$ and salt concentration. At $f_{EO,salt,}$ > 0.27, the addition of salt stabilizes the ordered phase; at $f_{EO,salt,}$ < 0.27, the addition of salt stabilizes the disordered phase. We propose a simple theoretical model to predict the block copolymer composition at which phase behavior is independent of salt concentration ($f_{EO,salt,}$ = 0.27). Here, we refer to this composition as the “isotaksis point”.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Colloquium: Ice rule and emergent frustration in particle ice and beyond

Geometric frustration and the ice rule are two concepts that are intimately connected and widespread across condensed matter. The first refers to the inability of a system to satisfy competing interactions in the presence of spatial constraints. The second, in its more general sense, represents a prescription for the minimization of the topological charges in a constrained system. Both can lead to manifolds of high susceptibility and nontrivial, constrained disorder where exotic behaviors can appear and even be designed deliberately. This Colloquium describes the emergence of geometric frustration and the ice rule in soft condensed matter. It excludes the extensive developments of mathematical physics within the field of geometric frustration, but rather focuses on systems of confined microscopic or mesoscopic particles that emerge as a novel paradigm exhibiting spin degrees of freedom. In such systems, geometric frustration can be engineered artificially by controlling the spatial topology and geometry of the lattice, the position of the individual particle units, or their relative filling fraction. These capabilities enable the creation of novel and exotic phases of matter and also potentially lead toward technological applications related to memory and logic devices that are based on the motion of topological defects. The rapid progress in theory and experiments is reviewed and the intimate physical connections with other frustrated systems at different length scales are discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

A high-mobility electronic system at an electrolyte-gated oxide surface

Electrolyte gating is a powerful technique for accumulating large carrier densities at a surface. Yet this approach suffers from significant sources of disorder: electrochemical reactions can damage or alter the sample, and the ions of the electrolyte and various dissolved contaminants sit Angstroms from the electron system. Accordingly, electrolyte gating is well suited to studies of superconductivity and other phenomena robust to disorder, but of limited use when reactions or disorder must be avoided. Here we demonstrate that these limitations can be overcome by protecting the sample with a chemically inert, atomically smooth sheet of hexagonal boron nitride. We illustrate our technique with electrolyte-gated strontium titanate, whose mobility when protected with boron nitride improves more than 10-fold while achieving carrier densities nearing 10 14 cm –2 . In conclusion, our technique is portable to other materials, and should enable future studies where high carrier density modulation is required but electrochemical reactions and surface disorder must be minimized.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Thermoelectricity in transition metal compounds: The role of spin disorder

Here, at room temperature and above, most magnetic materials adopt a spin-disordered (paramagnetic) state whose electronic properties can differ significantly from their low-temperature, spin-ordered counterparts. Yet computational searches for new functional materials usually assume some type of magnetic order. In the present work, we demonstrate a methodology to incorporate spin disorder in computational searches and predict the electronic properties of the paramagnetic phase. We implement this method in a high-throughput framework to assess the potential for thermoelectric performance of 1350 transition-metal sulfides and find that all magnetic systems we identify as promising in the spin-ordered ground state cease to be promising in the paramagnetic phase due to disorder-induced deterioration of the charge carrier transport properties. We also identify promising non-magnetic candidates that do not suffer from these spin disorder effects. In addition to identifying promising materials, our results offer insights into the apparent scarcity of magnetic systems among known thermoelectrics and highlight the importance of including spin disorder in computational searches.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Localization properties and high-fidelity state transfer in hopping models with correlated disorder

We investigate a tight-binding chain featuring diagonal and off-diagonal disorder, these being modeled through the long-range-correlated fractional Brownian motion. Particularly, by employing exact diagonalization methods, we evaluate how the eigenstate spectrum of the system and how its related single-particle dynamics respond to both competing sources of disorder. Moreover, we report the possibility of carrying out efficient end-to-end quantum-state transfer protocols even in the presence of such generalized disorder due to the appearance of extended states around the middle of the band in the limit of strong correlations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

NMR study of Ni 50+x ⁢Ti 50-x strain glasses

Here, we studied Ni 50+x ⁢Ti 50-x with compositions up to x = 2, performing 47 Ti and 49 Ti nuclear magnetic resonance (NMR) measurements from 4 to 400 K. For large x in this system, a strain glass appears in which frozen ferroelastic nanodomains replace the displacive martensite structural transition. Here, we demonstrate that NMR can provide an extremely effective probe of the strain-glass freezing process, with large changes in NMR line shape due to the effects of random strains which become motionally narrowed at high temperatures. At the same time with high-resolution x-ray diffraction we confirm the lack of structural changes in x ≥ 1.2 samples, while we show that there is little change in the electronic behavior across the strain-glass freezing temperature. NMR spin-lattice relaxation time (T 1 ) measurements provide a further measure of the dynamics of the freezing process, and indicate a predominantly thermally activated behavior both above and below the strain-glass freezing temperature. We show that the strain-glass results are consistent with a very small density of critically divergent domains undergoing a Vogel-Fulcher-type freezing process, coexisting with domains exhibiting faster dynamics and stronger pinning.

36 MATERIALS SCIENCE↗