Articles on the spot

Universal fragment descriptors for predicting properties of inorganic crystals

Olexandr Isayev, Corey Oses, Cormac Toher, Eric Gosset, Stefano Curtarolo and Alexander Tropsha

Although historically materials discovery has been driven by a laborious trial-and-error process, knowledge-driven materials design can now be enabled by the rational combination of Machine Learning methods and materials databases. Here, data from the AFLOW repository for ab initio calculations is combined with Quantitative Materials Structure-Property Relationship models to predict important properties: metal/insulator classification, band gap energy, bulk/shear moduli, Debye temperature and heat capacities. The prediction’s accuracy compares well with the quality of the training data for virtually any stoichiometric inorganic crystalline material, reciprocating the available thermomechanical experimental data. The universality of the approach is attributed to the construction of the descriptors: Property-Labelled Materials Fragments. The representations require only minimal structural input allowing straightforward implementations of simple heuristic design rules.

High-Throughput Computation of Thermal Conductivity of High-Temperature Solid Phases: The Case of Oxide and Fluoride Perovskitess

Ambroise van Roekeghem, Jesús Carrete, Corey Oses, Stefano Curtarolo, and Natalio Mingo

Using finite-temperature phonon calculations and machine-learning methods, we assess the mechanical stability of about 400 semiconducting oxides and fluorides with cubic perovskite structures at 0, 300, and 1000 K. We find 92 mechanically stable compounds at high temperatures—including 36 not mentioned in the literature so far—for which we calculate the thermal conductivity. We show that the thermal conductivity is generally smaller in fluorides than in oxides, largely due to a lower ionic charge, and describe simple structural descriptors that are correlated with its magnitude. Furthermore, we show that the thermal conductivities of most cubic perovskites decrease more slowly than the usual T-1 behavior. Within this set, we also screen for materials exhibiting negative thermal expansion. Finally, we describe a strategy to accelerate the discovery of mechanically stable compounds at high temperatures.

Spectral descriptors for bulk metallic glasses based on the thermodynamics of competing crystalline phases

Eric Perim, Dongwoo Lee, Yanhui Liu4, Cormac Toher, Pan Gong, Yanglin Li, W. Neal Simmons, Ohad Levy, Joost J. Vlassak, Jan Schroers, and Stefano Curtarolo

Metallic glasses attract considerable interest due to their unique combination of superb properties and processability. Predicting their formation from known alloy parameters remains the major hindrance to the discovery of new systems. Here, we propose a descriptor based on the heuristics that structural and energetic ‘confusion’ obstructs crystalline growth, and demonstrate its validity by experiments on two well-known glass-forming alloy systems. We then develop a robust model for predicting glass formation ability based on the geometrical and energetic features of crystalline phases calculated ab initio in the AFLOW framework. Our findings indicate that the formation of metallic glass phases could be much more common than currently thought, with more than 17% of binary alloy systems potential glass formers. Our approach pinpoints favourable compositions and demonstrates that smart descriptors, based solely on alloy properties available in online repositories, offer the sought-after key for accelerated discovery of metallic glasses.

Modeling Off-Stoichiometry Materials with a High-Throughput Ab-Initio Approach

Kesong Yang, CoreyOses, and Stefano Curtarolo

Predicting material properties of off-stoichiometry systems remains a long-standing and formidable challenge in rational materials design. A proper analysis of such systems by means of a supercell approach requires the exhaustive consideration of all possible superstructures, which can be a time-consuming process. On the contrary, the use of quasirandom approximants, although very computationally effective, implicitly bias the analysis toward disordered states with the lowest site correlations. Here, we propose a novel framework designed specifically to investigate stoichiometrically driven trends of disordered systems (i.e., having partial occupation and/or disorder in the atomic sites). At the heart of the approach is the identification and analysis of unique supercells of a virtually equivalent stoichiometry to the disordered material. We employ Boltzmann statistics to resolve system-wide properties at a high-throughput (HT) level. To maximize efficiency and accessibility, we integrated the method within the automatic HT computational framework AFLOW. As proof of concept, we apply our approach to three systems of interest, a zinc chalcogenide (ZnS1−xSex), a wide-gap oxide semiconductor (MgxZn1−xO), and an iron alloy (Fe1−xCux), at various stoichiometries. These systems exhibit properties that are highly tunable as a function of composition, characterized by optical bowing and linear ferromagnetic behavior. Not only are these qualities successfully predicted, but additional insight into underlying physical mechanisms is revealed.

Entropy Stabilized Oxides

C. M. Rost, E. Sachet, T. Borman, A. Moballegh, E. C. Dickey, D. Hou, J. L. Jones, S. Curtarolo, and J.-P. Maria

Configurational disorder can be compositionally engineered into mixed oxide by populating a single sublattice with many distinct cations. The formulations promote novel and entropy-stabilized forms of crystalline matter where metal cations are incorporated in new ways. Here, through rigorous experiments, a simple thermodynamic model, and a five-component oxide formulation, we demonstrate beyond reasonable doubt that entropy predominates the thermodynamic landscape, and drives a reversible solid-state transformation between a multiphase and single-phase state. In the latter, cation distributions are proven to be random and homogeneous. The findings validate the hypothesis that deliberate configurational disorder provides an orthogonal strategy to imagine and discover new phases of crystalline matter and untapped opportunities for property engineering.

Convergence of multi-valley bands as the electronic origin of high thermoelectric performance in CoSb3 skutterudites

Yinglu Tang, Zachary M. Gibbs, Luis A. Agapito, Guodong Li, Hyun-Sik Kim, Marco Buongiorno Nardelli, Stefano Curtarolo and G. Jeffrey Snyder

Filled skutterudites RixCo4Sb12 are excellent n-type thermoelectric materials owing to their high electronic mobility and higheffective mass, combined with low thermal conductivity associated with the addition of filler atoms into the void site. Thefavourable electronic band structure in n-type CoSb3 is typically attributed to threefold degeneracy at the conduction band minimum accompanied by linear band behaviour at higher carrier concentrations, which is thought to be related to the increase in effective mass as the doping level increases. Using combined experimental and computational studies, we show instead that a secondary conduction band with 12 conducting carrier pockets (which converges with the primary band at high temperatures) is responsible for the extraordinary thermoelectric performance of n-type CoSb3 skutterudites. A theoretical explanation is also provided as to why the linear (or Kane-type) band feature is not beneficial for thermoelectrics.

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