75 research outputs found
Method for locating low-energy solutions within DFT+U
The widely employed DFT+U formalism is known to give rise to many self-consistent yet energetically distinct solutions in correlated systems, which can be highly problematic for reliably predicting the thermodynamic and physical properties of such materials. Here we study this phenomenon in the bulk materials UO_2, CoO, and NiO, and in a CeO_2 surface. We show that the following factors affect which self-consistent solution a DFT+U calculation reaches: (i) the magnitude of U; (ii) initial correlated orbital occupations; (iii) lattice geometry; (iv) whether lattice symmetry is enforced on the charge density; and (v) even electronic mixing parameters. These various solutions may differ in total energy by hundreds of meV per atom, so identifying or approximating the ground state is critical in the DFT+U scheme. We propose an efficient U-ramping method for locating low-energy solutions, which we validate in a range of test cases. We also suggest that this method may be applicable to hybrid functional calculations
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High-Throughput Machine-Learning-Driven Synthesis of Full-Heusler Compounds
A machine-learning model has been trained to discover Heusler compounds, which are intermetallics exhibiting diverse physical properties attractive for applications in thermoelectric and spintronic materials. Improving these properties requires knowledge of crystal structures, which occur in three subtle variations (Heusler, inverse Heusler, and CsCl-type structures) that are difficult, and at times impossible, to distinguish by diffraction techniques. Compared to alternative approaches, this Heusler discovery engine performs exceptionally well, making fast and reliable predictions of the occurrence of Heusler vs non-Heusler compounds for an arbitrary combination of elements with no structural input on over 400 000 candidates. The model has a true positive rate of 0.94 (and false positive rate of 0.01). It is also valuable for data sanitizing, by flagging questionable entries in crystallographic databases. It was applied to screen candidates with the formula ABC and predict the existence of 12 novel gallides MRuGa and RuMGa (M = Ti-Co) as Heusler compounds, which were confirmed experimentally. One member, TiRuGa, exhibited diagnostic superstructure peaks that confirm the adoption of an ordered Heusler as opposed to a disordered CsCl-type structure
Small Polarons in Transition Metal Oxides
The formation of polarons is a pervasive phenomenon in transition metal oxide
compounds, with a strong impact on the physical properties and functionalities
of the hosting materials. In its original formulation the polaron problem
considers a single charge carrier in a polar crystal interacting with its
surrounding lattice. Depending on the spatial extension of the polaron
quasiparticle, originating from the coupling between the excess charge and the
phonon field, one speaks of small or large polarons. This chapter discusses the
modeling of small polarons in real materials, with a particular focus on the
archetypal polaron material TiO2. After an introductory part, surveying the
fundamental theoretical and experimental aspects of the physics of polarons,
the chapter examines how to model small polarons using first principles schemes
in order to predict, understand and interpret a variety of polaron properties
in bulk phases and surfaces. Following the spirit of this handbook, different
types of computational procedures and prescriptions are presented with specific
instructions on the setup required to model polaron effects.Comment: 36 pages, 12 figure
Benchmarking Materials Property Prediction Methods: The Matbench Test Set and Automatminer Reference Algorithm
We present a benchmark test suite and an automated machine learning procedure
for evaluating supervised machine learning (ML) models for predicting
properties of inorganic bulk materials. The test suite, Matbench, is a set of
13 ML tasks that range in size from 312 to 132k samples and contain data from
10 density functional theory-derived and experimental sources. Tasks include
predicting optical, thermal, electronic, thermodynamic, tensile, and elastic
properties given a materials composition and/or crystal structure. The
reference algorithm, Automatminer, is a highly-extensible, fully-automated ML
pipeline for predicting materials properties from materials primitives (such as
composition and crystal structure) without user intervention or hyperparameter
tuning. We test Automatminer on the Matbench test suite and compare its
predictive power with state-of-the-art crystal graph neural networks and a
traditional descriptor-based Random Forest model. We find Automatminer achieves
the best performance on 8 of 13 tasks in the benchmark. We also show our test
suite is capable of exposing predictive advantages of each algorithm - namely,
that crystal graph methods appear to outperform traditional machine learning
methods given ~10^4 or greater data points. The pre-processed, ready-to-use
Matbench tasks and the Automatminer source code are open source and available
online (http://hackingmaterials.lbl.gov/automatminer/). We encourage evaluating
new materials ML algorithms on the MatBench benchmark and comparing them
against the latest version of Automatminer.Comment: Main text, supplemental inf
Expanding frontiers in materials chemistry and physics with multiple anions
During the last century, inorganic oxide compounds laid foundations for materials synthesis, characterization, and technology translation by adding new functions into devices previously dominated by main-group element semiconductor compounds. Today, compounds with multiple anions beyond the single-oxide ion, such as oxyhalides and oxyhydrides, offer a new materials platform from which superior functionality may arise. Here we review the recent progress, status, and future prospects and challenges facing the development and deployment of mixed-anion compounds, focusing mainly on oxide-derived materials. We devote attention to the crucial roles that multiple anions play during synthesis, characterization, and in the physical properties of these materials. We discuss the opportunities enabled by recent advances in synthetic approaches for design of both local and overall structure, state-of-the-art characterization techniques to distinguish unique structural and chemical states, and chemical/physical properties emerging from the synergy of multiple anions for catalysis, energy conversion, and electronic materials
Expanded dataset of mechanical properties and observed phases of multi-principal element alloys
This data article presents a compilation of mechanical properties of 630 multi-principal element alloys (MPEAs). Built upon recently published MPEA databases, this article includes updated records from previous reviews (with minor error corrections) along with new data from articles that were published since 2019. The extracted properties include reported composition, processing method, microstructure, density, hardness, yield strength, ultimate tensile strength (or maximum compression strength), elongation (or maximum compression strain), and Young’s modulus. Additionally, descriptors (e.g. grain size) not included in previous reviews were also extracted for articles that reported them. The database is hosted and continually updated on an open data platform, Citrination. To promote interpretation, some data are graphically presented
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