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

Abstract

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.

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:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Next Generation of Materials by Design: Incorporating Metastability (CNGMD); National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1462337
Alternate Identifier(s):
OSTI ID: 1429571
Report Number(s):
NREL/JA-5K00-72058
Journal ID: ISSN 2475-9953; PRMHAR; TRN: US1902143
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Journal Article: 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)
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

Citation Formats

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., 2018. 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. https://doi.org/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. https://doi.org/10.1103/PhysRevMaterials.2.033802. https://www.osti.gov/servlets/purl/1462337.
@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},
url = {https://www.osti.gov/biblio/1462337}, journal = {Physical Review Materials},
issn = {2475-9953},
number = 3,
volume = 2,
place = {United States},
year = {Mon Mar 26 00:00:00 EDT 2018},
month = {Mon Mar 26 00:00:00 EDT 2018}
}

Journal Article:

Citation Metrics:
Cited by: 11 works
Citation information provided by
Web of Science

Figures / Tables:

FIG. 1. FIG. 1. : Schematics of the two step, structure mapping algorithm developed in this work (see text for details).

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.