Evolutionary Crystal Structure Prediction as a Method for the Discovery of Minerals and Materials

Oganov, Artem R.; Ma, Yanming; Lyakhov, Andriy O.; Valle, M.; Gatti, Carlo

doi:10.2138/rmg.2010.71.13

Cited by 200 publications

(136 citation statements)

References 87 publications

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“…However, we found that the formation of this phase is impeded, which explain the observed previously dependence of T c on the experimental P-T path [7,8]. The experiments have been combined with theoretical variable composition searches using USPEX code [20] …”

Section: Introductionmentioning

confidence: 62%

“…Predictions of stable phases were done using the USPEX code in the variable-composition mode [20] at 0, 30, 60, 90, 120, 140 GPa. The first generation of structures (up to 32 atoms per the primitive cell) was produced randomly and the succeeding generations were obtained by applying heredity, atom transmutation, softmutation, and random variational operators, with probabilities of 40%, 20%, 20%, and 20%, respectively.…”

Section: Experimental and Computational Methodsmentioning

confidence: 99%

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Hydrogen sulfide at high pressure: Change in stoichiometry

et al. 2016

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Section: Introductionmentioning

confidence: 62%

Section: Experimental and Computational Methodsmentioning

confidence: 99%

Hydrogen sulfide at high pressure: Change in stoichiometry

et al. 2016

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“…Predictions of stable phases were done using the USPEX code in the variable-composition mode [30]. The first generation of structures was produced randomly and the succeeding generations were obtained by applying heredity, atom transmutation, and lattice mutation operations, with probabilities of 60%, 10% and 30%, respectively.…”

Section: Methodsmentioning

confidence: 99%

Backbone NxH compounds at high pressures

Goncharov

Holtgrewe

Qian

et al. 2015

The Journal of Chemical Physics

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Optical and synchrotron x-ray diffraction diamond anvil cell experiments have been combined with first principles theoretical structure predictions to investigate mixed N 2 and H 2 up to 55 GPa. We found the formation of oligomeric N x H (x1) compounds using mechano-and photochemistry at pressures above 47 and 10 GPa, respectively, and room temperature. These compounds can be recovered to ambient pressure at T<130 K, whereas at room temperature, they can be metastable down to 3.5 GPa. Our results suggest new pathways for synthesis of environmentally benign high energy-density materials and alternative planetary ice.

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“…Therefore, knowledge not only of average liquid configurations but also of the solid mixture's structure is essential. For phase transitions of mixtures, the problem is hence strongly linked to the challenge of predicting molecular crystals from first principles [12], which has been addressed for co-crystals only recently [7,13] in mapping out entire phase diagrams. For the identification of HTF mixtures with minimal melting points, however, it is sufficient to simply focus on eutectics, rather than having to screen the entire solid-liquid phase diagram.…”

mentioning

confidence: 99%

“…Therefore, knowledge not only of average liquid configurations but also of the solid mixture's structure is essential. For phase transitions of mixtures, the problem is hence strongly linked to the challenge of predicting molecular crystals from first principles [12], which has been addressed for co-crystals only recently [7,13]. Recent efforts to compute solid-liquid phase equilibria of hard sphere mixtures [14], Lennard-Jones mixtures [15], alloys [16], or solid and liquid mixtures of the Rb/Cs fluoride binary [17] in mapping out entire phase diagrams.…”

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confidence: 99%

Molten salt eutectics from atomistic simulations

2011

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Despite their importance for solar thermal power applications, phase-diagrams of molten salt mixture heat transfer fluids (HTFs) are not readily accessible from first principles. We present a molecular dynamics scheme general enough to identify eutectics of any HTF candidate mixture. The eutectic mixture and temperature are located using the liquid mixture free energy and the pure component solid-liquid free energy differences. The liquid mixture free energy is obtained using thermodynamic integration over particle identity transmutations sampled with molecular dynamics at a single temperature. According to Carnot's cycle, the maximum efficiency of solar thermal power facilities increases with the temperature difference between melting and thermal decomposition of employed heat transfer fluids (HTFs). Consequently, new formulations of low melting but temperature resistant molten salt mixtures are actively sought [1]. Competitive formulations currently include eutectics of alkali and alkali-metal earth nitrates and nitrite mixtures. Unfortunately, the dimensionality of the combinatorial multicomponent space of all possible cations and anions prohibits exhaustive scanning using computer simulation. Once an optimal HTF formulation is identified, however, its realization through simple mixing is readily accomplished in experiment. Identifying new HTFs therefore represents a rewarding challenge for atomistic first principles materials design efforts using theory and computation. Ab initio (AI) based design, through an efficient combination of first principles methods and optimization algorithms [2], has already been applied to inverting band structures [3], identifying stable alloys [4], designing heterogeneous catalysts [5,6], or discovering ternary metal oxides for batteries [7]. Identity transformations, also called "alchemical" transmutations [8], have been successfully applied to compute compositions in the earth's core [9], phase stability in solid solutions [10], and a wide variety of biochemical applications [11], among others.The Gibbs criteria for phase equilibrium dictates that temperature, pressure, and chemical potential of individual components must be equal in coexisting phases. Therefore, knowledge not only of average liquid configurations but also of the solid mixture's structure is essential. For phase transitions of mixtures, the problem is hence strongly linked to the challenge of predicting molecular crystals from first principles [12], which has been addressed for co-crystals only recently [7,13] in mapping out entire phase diagrams. For the identification of HTF mixtures with minimal melting points, however, it is sufficient to simply focus on eutectics, rather than having to screen the entire solid-liquid phase diagram. Here, we present a first principles approach for directly estimating eutectic compositions and temperatures for any number of components, relying on a combination of only a couple of molecular dynamics (MD) calculations per mole fraction at a single temperature and knowledge ab...

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Evolutionary Crystal Structure Prediction as a Method for the Discovery of Minerals and Materials

Cited by 200 publications

References 87 publications

Hydrogen sulfide at high pressure: Change in stoichiometry

Hydrogen sulfide at high pressure: Change in stoichiometry

Backbone NxH compounds at high pressures

Molten salt eutectics from atomistic simulations

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