The glassy solid as a statistical ensemble of crystalline microstates
Abstract
We present an alternative and, for the purpose of non-crystalline materials design, a more suitable description of covalent and ionic glassy solids as statistical ensembles of crystalline local minima on the potential energy surface. Motivated by the concept of partially broken ergodicity, we analytically formulate the set of approximations under which the structural features of ergodic systems such as the radial distribution function (RDF) and powder X-ray diffraction (XRD) intensity can be rigorously expressed as statistical ensemble averages over different local minima. Validation is carried out by evaluating these ensemble averages for elemental Si and SiO2 over the local minima obtained through the first-principles random structure sampling that we performed using relatively small simulation cells, thereby restricting the sampling to a set of predominantly crystalline structures. The comparison with XRD and RDF from experiments (amorphous silicon) and molecular dynamics simulations (glassy SiO2) shows excellent agreement, thus supporting the ensemble picture of glasses and opening the door to fully predictive description without the need for experimental inputs.
- Publication Date:
- Research Org.:
- National Renewable Energy Laboratory (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Institutes of Heath (NIH)
- OSTI Identifier:
- 1618518
- Alternate Identifier(s):
- OSTI ID: 1660018
- Report Number(s):
- NREL/JA-5K00-77246
Journal ID: ISSN 2057-3960; 56; PII: 329
- Grant/Contract Number:
- AC36-08GO28308; T32-GM008759; SC0014664; SC0019306
- Resource Type:
- Published Article
- Journal Name:
- npj Computational Materials
- Additional Journal Information:
- Journal Name: npj Computational Materials Journal Volume: 6 Journal Issue: 1; Journal ID: ISSN 2057-3960
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; atomistic models; structure of solids and liquids
Citation Formats
Jones, Eric B., and Stevanović, Vladan. The glassy solid as a statistical ensemble of crystalline microstates. United Kingdom: N. p., 2020.
Web. doi:10.1038/s41524-020-0329-2.
Jones, Eric B., & Stevanović, Vladan. The glassy solid as a statistical ensemble of crystalline microstates. United Kingdom. https://doi.org/10.1038/s41524-020-0329-2
Jones, Eric B., and Stevanović, Vladan. Thu .
"The glassy solid as a statistical ensemble of crystalline microstates". United Kingdom. https://doi.org/10.1038/s41524-020-0329-2.
@article{osti_1618518,
title = {The glassy solid as a statistical ensemble of crystalline microstates},
author = {Jones, Eric B. and Stevanović, Vladan},
abstractNote = {We present an alternative and, for the purpose of non-crystalline materials design, a more suitable description of covalent and ionic glassy solids as statistical ensembles of crystalline local minima on the potential energy surface. Motivated by the concept of partially broken ergodicity, we analytically formulate the set of approximations under which the structural features of ergodic systems such as the radial distribution function (RDF) and powder X-ray diffraction (XRD) intensity can be rigorously expressed as statistical ensemble averages over different local minima. Validation is carried out by evaluating these ensemble averages for elemental Si and SiO2 over the local minima obtained through the first-principles random structure sampling that we performed using relatively small simulation cells, thereby restricting the sampling to a set of predominantly crystalline structures. The comparison with XRD and RDF from experiments (amorphous silicon) and molecular dynamics simulations (glassy SiO2) shows excellent agreement, thus supporting the ensemble picture of glasses and opening the door to fully predictive description without the need for experimental inputs.},
doi = {10.1038/s41524-020-0329-2},
journal = {npj Computational Materials},
number = 1,
volume = 6,
place = {United Kingdom},
year = {Thu May 14 00:00:00 EDT 2020},
month = {Thu May 14 00:00:00 EDT 2020}
}
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/s41524-020-0329-2
https://doi.org/10.1038/s41524-020-0329-2
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 12 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
High Resolution Radial Distribution Function of Pure Amorphous Silicon
journal, April 1999
- Laaziri, Khalid; Kycia, S.; Roorda, S.
- Physical Review Letters, Vol. 82, Issue 17
Molecular Dynamics Simulation of Amorphous SiO 2 Nanoparticles
journal, November 2007
- Hoang, Vo Van
- The Journal of Physical Chemistry B, Vol. 111, Issue 44
Potential energy surface of monatomic liquids
journal, August 2018
- Sjostrom, Travis; De Lorenzi-Venneri, Giulia; Wallace, Duane C.
- Physical Review B, Vol. 98, Issue 5
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Density of amorphous Si
journal, January 1994
- Custer, J. S.; Thompson, Michael O.; Jacobson, D. C.
- Applied Physics Letters, Vol. 64, Issue 4
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Beyond sixfold coordinated Si in SiO 2 glass at ultrahigh pressures
journal, September 2017
- Prescher, Clemens; Prakapenka, Vitali B.; Stefanski, Johannes
- Proceedings of the National Academy of Sciences, Vol. 114, Issue 38
Genesis of concepts on structure of inorganic glasses
journal, August 1990
- Porai-Koshits, E. A.
- Journal of Non-Crystalline Solids, Vol. 123, Issue 1-3
On the nanostructure of pure amorphous silicon
journal, July 1995
- Williamson, D. L.; Roorda, S.; Chicoine, M.
- Applied Physics Letters, Vol. 67, Issue 2
Ising model phase-diagram calculations in the fcc lattice with first- and second-neighbor interactions
journal, February 1982
- Sanchez, J. M.; de Fontaine, D.
- Physical Review B, Vol. 25, Issue 3
Spectral descriptors for bulk metallic glasses based on the thermodynamics of competing crystalline phases
journal, August 2016
- Perim, Eric; Lee, Dongwoo; Liu, Yanhui
- Nature Communications, Vol. 7, Issue 1
Sampling Polymorphs of Ionic Solids using Random Superlattices
journal, February 2016
- Stevanović, Vladan
- Physical Review Letters, Vol. 116, Issue 7
Formation of thin-film crystalline silicon on glass observed by in-situ XRD
journal, August 2010
- Westra, J. M.; Vavruňková, V.; Šutta, P.
- Energy Procedia, Vol. 2, Issue 1
Ideal Glass States Are Not Purely Vibrational: Insight from Randomly Pinned Glasses
journal, November 2018
- Ozawa, Misaki; Ikeda, Atsushi; Miyazaki, Kunimasa
- Physical Review Letters, Vol. 121, Issue 20
Generalized cluster description of multicomponent systems
journal, November 1984
- Sanchez, J. M.; Ducastelle, F.; Gratias, D.
- Physica A: Statistical Mechanics and its Applications, Vol. 128, Issue 1-2
Optimal atomic structure of amorphous silicon obtained from density functional theory calculations
journal, June 2017
- Pedersen, Andreas; Pizzagalli, Laurent; Jónsson, Hannes
- New Journal of Physics, Vol. 19, Issue 6
Properties of a Continuous-Random-Network Model for Amorphous Systems
journal, November 1998
- Tu, Yuhai; Tersoff, J.; Grinstein, G.
- Physical Review Letters, Vol. 81, Issue 22
Non-crystalline solids: glasses and amorphous solids
journal, February 1996
- Gupta, Prabhat K.
- Journal of Non-Crystalline Solids, Vol. 195, Issue 1-2
Field Theory for Amorphous Solids
journal, September 2018
- DeGiuli, E.
- Physical Review Letters, Vol. 121, Issue 11
Cluster expansion made easy with Bayesian compressive sensing
journal, October 2013
- Nelson, Lance J.; Ozoliņš, Vidvuds; Reese, C. Shane
- Physical Review B, Vol. 88, Issue 15
Polymorphism in elemental silicon: Probabilistic interpretation of the realizability of metastable structures
journal, November 2017
- Jones, Eric B.; Stevanović, Vladan
- Physical Review B, Vol. 96, Issue 18
In Situ XRD and Electrochemical Study of the Reaction of Lithium with Amorphous Silicon
journal, January 2004
- Hatchard, T. D.; Dahn, J. R.
- Journal of The Electrochemical Society, Vol. 151, Issue 6
Densities of amorphous Si films by nuclear backscattering
journal, October 1972
- Brodsky, M. H.; Kaplan, D.; Ziegler, J. F.
- Applied Physics Letters, Vol. 21, Issue 7
The configurational energy gap between amorphous and crystalline silicon
journal, September 2011
- Kail, F.; Farjas, J.; Roura, P.
- physica status solidi (RRL) - Rapid Research Letters, Vol. 5, Issue 10-11
Optimal allocation of replicas in parallel tempering simulations
journal, January 2005
- Rathore, Nitin; Chopra, Manan; de Pablo, Juan J.
- The Journal of Chemical Physics, Vol. 122, Issue 2
Statistical mechanics of glass
journal, August 2014
- Mauro, John C.; Smedskjaer, Morten M.
- Journal of Non-Crystalline Solids, Vol. 396-397