Bulletin of the American Physical Society
APS March Meeting 2019
Volume 64, Number 2
Monday–Friday, March 4–8, 2019; Boston, Massachusetts
Session Y19: Computational Materials Design and Discovery -- Synthesizability and Stability |
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Sponsoring Units: DMP DCOMP Chair: Eric Isaacs, Northwestern University Room: BCEC 156C |
Friday, March 8, 2019 11:15AM - 11:27AM |
Y19.00001: Networks of materials: a complexity approach to material synthesizability Muratahan Aykol, Vinay I Hegde, Santosh Suram, Linda Hung, Patrick Herring, Christopher Wolverton, Jens Hummelshøj Network science can provide a new arsenal of methods for materials informatics to address some of the daunting challenges in the field of materials.[1,2] One such challenge we address in this talk is the laboratory synthesis of computationally designed materials. The art of synthesis itself is too complex to be treated with an all-encompassing, quantitative approach as yet, because it involves not only the modeling of the energy landscape of competing phases or the kinetics of transformations, but also abstract factors, such as experience of scientists, state-of-the-art in experimental methods, resources and more. We present one of the first examples of “networks of materials” in the form of thermodynamic equilibria derived from high-throughput computational phase diagrams and analyze the local and global properties of this network.[1] We discuss how synthesis probabilities of yet-to-be-made, novel inorganic materials can be predicted from the dynamics of this network via machine-learning, connecting high-throughput computational design and experiments. |
Friday, March 8, 2019 11:27AM - 11:39AM |
Y19.00002: Roadmap for the Synthesis of Exotic 2D Metastable Carbon using Topologically Assembled Precursors Purusottam Jena, Hong Fang Metastable structures of matter often possess properties superior to those of their ground state. A case in point is diamond vs. graphite. Yet, many predicted metastable structures are dismissed as hard-to-realize in practice as their basins of attraction are either too shallow or too narrow or both. There is no available theoretical approach that can deliberately enhance the realizability of these structures and directly guide their experimental synthesis. Here, we introduce a new approach to create potential energy surfaces in which the volumes of the basin of attraction of targeted metastable structures are increased by design, while simultaneously suppressing the accessibility of the ground state as well as other isomers.This approach is based on topologically assembled precursors, followed by density functional theory relaxations,and is applied to realize high-energy carbon allotropes such as penta-graphene comprised entirely of pentagon rings, O-graphene comprised of five- and eight-membered rings and R-graphene comprised of four-, six- and eight-membered rings. |
Friday, March 8, 2019 11:39AM - 11:51AM |
Y19.00003: Disorder drives synthesizability of multi-component systems Cormac Toher, Corey Oses, Stefano Curtarolo The factorial increase in the number of potential compositions with increasing number of elemental components is not reflected in the number of synthesized ordered chemical compounds [1]. We show that this is due to formation-entropy-gain exceeding formation-enthalpy-gain as more species are added to the mixture. An analysis of the dependence of formation enthalpy on the number of species [2] using data extracted from the AFLOW data repository [3] shows interesting trends about the interplay between entropic and enthalpic effects on the synthesizability of multi-component materials. |
Friday, March 8, 2019 11:51AM - 12:03PM |
Y19.00004: Retrosynthetic Planning with Generative Models Shintaro Fukushima, Yuichi Motoyama, Kazuyoshi Yoshimi Recently, retrosynthetic planning with machine learning and deep learning has been studied actively. One of the powerful approach was the retrosynthesis based on the molecular similarity proposed by Coley et al. In this approach, similarities between the target product and products in the reaction database were calculated to find similar products. Next, candidate reactions were generated by modifying reactions of the similar targets. This method by Coley et al. is more accurate than other methods. However, its search space is limited because it is based on the matching with the existing reactions. |
Friday, March 8, 2019 12:03PM - 12:15PM |
Y19.00005: Fantastic Metastable States and Where to Find Them: A Computational Search for Superlattices with Enhanced Functional Properties John Bonini, Karin Rabe Superlattice systems continue to be of great interest in the development of new or enhanced material functionalities. One exciting prospect is that the conditions of the superlattice allow for the stabilization of novel states not accessible in bulk materials. To find such states, and the conditions under which they are stabilized, we construct a database of first principles calculations which describe not only the ground state of each constituent material, but a number of local minima and how these states change with mechanical, electrical, and other conditions. A data-driven approach is used in structure determination where the most probable local minima are systematically identified through analysis of existing materials databases. The resulting data set can be used as input to the "bulk-layer model" [1] to rapidly identify superlattice combinations with desirable functional properties, as well as the superlattice "stacking method" [2] to carefully compute the ground state of a particular superlattice. Examples applying the method to perovskite oxide compounds and superlattices will be presented. |
Friday, March 8, 2019 12:15PM - 12:27PM |
Y19.00006: Evaluating Species Stability with First Principles Calculations Lauren Walters, Liang-Feng Huang, James M Rondinelli Novel multicomponent materials such as BiCuOS and BiCuOSe are used in a wide variety of applications like structural materials, semiconductors, and catalysis; however, the complex chemistry of having multiple anions makes reliable synthesis of these products challenging. Here we describe an ab-initio approach to evaluate the thermodynamic stabilities of multicomponent solids in aqueous environments with variable environmental conditions. The approach allows us to generate electrochemical Pourbaix diagrams that can be used to guide hydrothermal synthesis of these complex phases. Furthermore, we utilize a revised Helgeson-Kirkham-Flowers model to incorporate nonstandard state conditions for aqueous ions as functions of temperature and pressure. Our work identifies the main factors needed for the informed synthesis of new complex transition metal compounds and routes to deliver long-term stability of copper-based alloys. |
Friday, March 8, 2019 12:27PM - 12:39PM |
Y19.00007: Formation enthalpies for automated computational materials design Rico Friedrich, Demet Usanmaz, Corey Oses, Andrew R Supka, Marco Fornari, Marco Buongiorno Nardelli, Cormac Toher, Stefano Curtarolo The accurate calculation of formation enthalpies is crucial for computational materials design. For compounds chemically similar to their reference phases such as metal alloys, standard semi-local approximations to density functional theory (DFT) lead to accurate results [1]. When the phases are chemically dissimilar as in the case of oxides, DFT suffers from a lack of error cancellation leading to deviations of several hundred meV/atom compared to experimental values [2]. We use the automated computational materials design framework AFLOW [3] to benchmark correction schemes for ab initio formation enthalpies [2, 4]. These empirical methods can improve DFT predictions by a factor of 4 to 7. Zero-point vibrational and thermal contributions to the formation enthalpy are found to largely cancel each other. |
Friday, March 8, 2019 12:39PM - 12:51PM |
Y19.00008: The Phase Stability Network of All Inorganic Materials Vinay Ishwar Hegde, Muratahan Aykol, Christopher Wolverton In the pursuit of unlocking structure-property relationships, a dominant paradigm in materials science has been the bottom-up investigation of how the arrangement of atoms and interatomic bonding in a material determine its macroscopic behavior. Here we consider a complementary approach, a top-down study of the organizational structure of networks of materials, based on the interaction between materials themselves. We unravel the "phase stability network of all inorganic materials" as a dense complex network of 21,000 thermodynamically stable compounds (nodes) connected with 41 million tie-lines (edges) defining their two-phase equilibria as computed by high-throughput density functional theory. The connectivity of nodes in the materials network shows a lognormal distribution, while the network itself shows small-world behavior, with a number of compounds acting as "hubs" having connections to nearly all other compounds. Analyzing the structure and topology of the materials network has the potential to uncover new knowledge inaccessible from the traditional atoms-to-materials approaches. We use the connectedness of materials in the network to derive a general, data-driven metric for reactivity, the "nobility index", and quantitatively identify the noblest materials in nature. |
Friday, March 8, 2019 12:51PM - 1:03PM |
Y19.00009: Instabilities during solid-solid structural phase transformations provide guidance for the high-throughput materials discovery Nikolai A Zarkevich, Hao Chen, Valery Levitas, Vitalij K Pecharsky, Duane D Johnson Electronic and lattice instabilities are studied during the solid-solid phase transformations in materials subjected to a general stress. The elastic instability criterion is proposed. The instability criteria are useful for the high-throughput discovery of novel materials. Our findings reveal novel, more practical synthesis routes for new or known high-pressure phases under predictable nonhydrostatic loading, where competition of instabilities can serve for phase selection. |
Friday, March 8, 2019 1:03PM - 1:15PM |
Y19.00010: Exploring the landscape of nonlinear mechanical metamaterials Eder Medina, Patrick Farrell, Christopher Rycroft, Katia Bertoldi Nonlinearities have recently emerged as a powerful tool for designing mechanical metamaterials, as they lead to systems with a complex and programmable response. Currently, nonlinear responses have primarily been explored through traditional experimental techniques and standard single-solution numerical solvers. Here, we use an in silico continuation method to discover multiple configurations with associated different properties for a single loading parameter. We test the method on simple porous structures under compressive loading; as the load increases, we discover bifurcating families of stable and metastable states. Using this method we find structures that can switch between energy-releasing and energy-harvesting configurations, and structures that are geometrically hysteretic. Physical experiments are conducted to validate the results. |
Friday, March 8, 2019 1:15PM - 1:27PM |
Y19.00011: Expanding the elemental space of atomic laminates by a theoretical/experimental approach Martin Dahlqvist, Johanna Rosen More than 50 years ago a family of atomically laminated compounds were discovered, being comprised of a transition metal M, an A-group element, and carbon and/or nitrogen X, and therefore being referred to as MAX phases. The exploration of the taxonomy of these can be accelerated by theoretical design on the atomic level combined with combinatorial experimental synthesis. Here, we use predictive phase stability calculations to probe transition metal (M) alloying in MAX phases and identify several chemically ordered structures. Subsequent materials synthesis of these indicates a potentially large family of thermodynamically stable phases, with Kagomé-like and in-plane chemical ordering, and with incorporation of elements previously not used for MAX phases, including Y and W. In extension, we suggest a matching set of novel two-dimensional MXenes, from selective etching of the A-element and, when so required, the alloying metal. The here demonstrated structural design on both 3D and 2D atomic levels expands the property tuning potential of functional ceramics. |
Friday, March 8, 2019 1:27PM - 1:39PM |
Y19.00012: Symmetry induced stability in alkali doped calcium-silicate-hydrate Ongun Ozcelik, Nishant Garg, Claire White CO2 emissions originating from the construction industry have a significant impact on global warming where the production of ordinary Portland cement clinker is responsible for approximately 8% of all human-made CO2. Alkali doped calcium-silicate-hydrate (C-S-H) is a critical silicate material since the use of blended cements and alkali-activated materials in construction industry can substantially reduce human-made CO2 emissions. However, the effect of alkali doping (Na and K) on the long-term stability and associated durability of C-S-H remains an open question. Here, using first principles quantum chemistry calculations on the model crystalline phase clinotobermorite, we show that there is a strong interplay between the thermodynamic stability of alkali doped C-S-H and the symmetry of the alkali atoms in the structure. We investigate the associated structural mechanisms by calculating the migration barriers of alkali atoms within the material, the electronic charge distribution in the material and the variation of basal spacing by using both computational methods and X-ray diffraction analysis. |
Friday, March 8, 2019 1:39PM - 1:51PM |
Y19.00013: Computational investigation of sulfosalts Ivor Loncaric, Predrag Lazic, Denis K Sunko Sulfosalts form a vast mineral group which may be imagined as chemically analogous to oxides, with O replaced by S. However, the metal cations in sulfosalts generally have tetrahedral S coordination, and the chemical variety is much greater than in oxides, owing to the several possible oxidation states of sulfur. Structurally they range from the very simple to the very complex, and also span the whole range of anisotropies, from chainlike to fully 3D. They are less ionic than oxides, thus they display surprising crystallochemical flexibility and superior tunability of the valence of the transition metal ions. This results in a large variety of interesting electronic, magnetic and mechanical properties. Here we present an initial study of a particular class of sulfosalts, based on murunskite. The electronic structure is discussed with respect to possible signatures of thermoelectricity and superconductivity. |
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