Polymorphism in elemental silicon: Probabilistic interpretation of the realizability of metastable structures
Abstract
With few systems of technological interest having been studied as extensively as elemental silicon, there currently exists a wide disparity between the number of predicted low-energy silicon polymorphs and those that have been experimentally realized as metastable at ambient conditions. We put forward an explanation for this disparity wherein the likelihood of formation of a given polymorph under near-equilibrium conditions can be estimated on the basis of mean-field isothermal-isobaric (N,p,T) ensemble statistics. The probability that a polymorph will be experimentally realized is shown to depend upon both the hypervolume of that structure's potential energy basin of attraction and a Boltzmann factor weight containing the polymorph's potential enthalpy per particle. Both attributes are calculated using density functional theory relaxations of randomly generated initial structures. We find that the metastable polymorphism displayed by silicon can be accounted for using this framework to the exclusion of a very large number of other low-energy structures.
- Authors:
-
- Colorado School of Mines, Golden, CO (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Next Generation of Materials by Design: Incorporating Metastability (CNGMD); National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1416520
- Alternate Identifier(s):
- OSTI ID: 1408170
- Report Number(s):
- NREL/JA-5K00-70758
Journal ID: ISSN 2469-9950; PRBMDO
- Grant/Contract Number:
- AC36-08GO28308
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 96; Journal Issue: 18; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; elemental silicon; polymorphism; metastable structures
Citation Formats
Jones, Eric B., and Stevanović, Vladan. Polymorphism in elemental silicon: Probabilistic interpretation of the realizability of metastable structures. United States: N. p., 2017.
Web. doi:10.1103/PhysRevB.96.184101.
Jones, Eric B., & Stevanović, Vladan. Polymorphism in elemental silicon: Probabilistic interpretation of the realizability of metastable structures. United States. https://doi.org/10.1103/PhysRevB.96.184101
Jones, Eric B., and Stevanović, Vladan. Fri .
"Polymorphism in elemental silicon: Probabilistic interpretation of the realizability of metastable structures". United States. https://doi.org/10.1103/PhysRevB.96.184101. https://www.osti.gov/servlets/purl/1416520.
@article{osti_1416520,
title = {Polymorphism in elemental silicon: Probabilistic interpretation of the realizability of metastable structures},
author = {Jones, Eric B. and Stevanović, Vladan},
abstractNote = {With few systems of technological interest having been studied as extensively as elemental silicon, there currently exists a wide disparity between the number of predicted low-energy silicon polymorphs and those that have been experimentally realized as metastable at ambient conditions. We put forward an explanation for this disparity wherein the likelihood of formation of a given polymorph under near-equilibrium conditions can be estimated on the basis of mean-field isothermal-isobaric (N,p,T) ensemble statistics. The probability that a polymorph will be experimentally realized is shown to depend upon both the hypervolume of that structure's potential energy basin of attraction and a Boltzmann factor weight containing the polymorph's potential enthalpy per particle. Both attributes are calculated using density functional theory relaxations of randomly generated initial structures. We find that the metastable polymorphism displayed by silicon can be accounted for using this framework to the exclusion of a very large number of other low-energy structures.},
doi = {10.1103/PhysRevB.96.184101},
journal = {Physical Review B},
number = 18,
volume = 96,
place = {United States},
year = {Fri Nov 03 00:00:00 EDT 2017},
month = {Fri Nov 03 00:00:00 EDT 2017}
}
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Works referencing / citing this record:
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