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Title: Predicting kinetics of polymorphic transformations from structure mapping and coordination analysis

To extend materials design and discovery into the space of metastable polymorphs, rapid and reliable assessment of transformation kinetics to lower energy structures is essential. Herein we focus on diffusionless polymorphic transformations and investigate routes to assess their kinetics using solely crystallographic arguments. As part of this investigation we developed a general algorithm to map crystal structures onto each other, and ascertain the low-energy (fast-kinetics) transformation pathways between them. Pathways with minimal dissociation of chemical bonds, along which the number of bonds (in ionic systems the first-shell coordination) does not decrease below that in the end structures, are shown to always be the fast-kinetics pathways. These findings enable the rapid assessment of the kinetics of polymorphic transformation and the identification of long-lived metastable structures. In conclusion, the utility is demonstrated on a number of transformations including those between high-pressure SnO 2 phases, which lack a detailed atomic-level understanding.
Authors:
 [1] ;  [2] ;  [2] ;  [3] ;  [4] ;  [5]
  1. Colorado School of Mines, Golden, CO (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. Univ. of Colorado, Boulder, CO (United States)
  3. Colorado School of Mines, Golden, CO (United States)
  4. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
  5. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Report Number(s):
NREL/JA-5K00-72058
Journal ID: ISSN 2475-9953; PRMHAR
Grant/Contract Number:
AC36-08GO28308
Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 2; Journal Issue: 3; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Research Org:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; phase transitions; specific phase transitions; solid-solid transformations
OSTI Identifier:
1462337
Alternate Identifier(s):
OSTI ID: 1429571

Stevanović, Vladan, Trottier, Ryan, Musgrave, Charles, Therrien, Félix, Holder, Aaron, and Graf, Peter. Predicting kinetics of polymorphic transformations from structure mapping and coordination analysis. United States: N. p., Web. doi:10.1103/PhysRevMaterials.2.033802.
Stevanović, Vladan, Trottier, Ryan, Musgrave, Charles, Therrien, Félix, Holder, Aaron, & Graf, Peter. Predicting kinetics of polymorphic transformations from structure mapping and coordination analysis. United States. doi:10.1103/PhysRevMaterials.2.033802.
Stevanović, Vladan, Trottier, Ryan, Musgrave, Charles, Therrien, Félix, Holder, Aaron, and Graf, Peter. 2018. "Predicting kinetics of polymorphic transformations from structure mapping and coordination analysis". United States. doi:10.1103/PhysRevMaterials.2.033802.
@article{osti_1462337,
title = {Predicting kinetics of polymorphic transformations from structure mapping and coordination analysis},
author = {Stevanović, Vladan and Trottier, Ryan and Musgrave, Charles and Therrien, Félix and Holder, Aaron and Graf, Peter},
abstractNote = {To extend materials design and discovery into the space of metastable polymorphs, rapid and reliable assessment of transformation kinetics to lower energy structures is essential. Herein we focus on diffusionless polymorphic transformations and investigate routes to assess their kinetics using solely crystallographic arguments. As part of this investigation we developed a general algorithm to map crystal structures onto each other, and ascertain the low-energy (fast-kinetics) transformation pathways between them. Pathways with minimal dissociation of chemical bonds, along which the number of bonds (in ionic systems the first-shell coordination) does not decrease below that in the end structures, are shown to always be the fast-kinetics pathways. These findings enable the rapid assessment of the kinetics of polymorphic transformation and the identification of long-lived metastable structures. In conclusion, the utility is demonstrated on a number of transformations including those between high-pressure SnO2 phases, which lack a detailed atomic-level understanding.},
doi = {10.1103/PhysRevMaterials.2.033802},
journal = {Physical Review Materials},
number = 3,
volume = 2,
place = {United States},
year = {2018},
month = {3}
}

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
  • DOI: 10.1103/PhysRevLett.77.3865

Projector augmented-wave method
journal, December 1994

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996

A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000
  • Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes
  • The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904
  • DOI: 10.1063/1.1329672