Chemical and Lattice Stability of the Tin Sulfides
File(s)1703.00361.pdf (3.06 MB)
Accepted version
OA Location
Author(s)
Skelton, JM
Burton, LA
Oba, F
Walsh, A
Type
Journal Article
Abstract
The tin sulfides represent a materials platform for earth-abundant semiconductor technologies. We present a first-principles study of the five known and proposed phases of SnS together with SnS2 and Sn2S3. Lattice-dynamics techniques are used to evaluate the dynamical stability and temperature-dependent thermodynamic free energy, and we also consider the effect of dispersion forces on the energetics. The recently identified π-cubic phase of SnS is found to be metastable with respect to the well-known orthorhombic Pnma/Cmcm equilibrium. The Cmcm phase is a low-lying saddle point between Pnma local minima on the potential-energy surface and is observed as an average structure at high temperatures. Bulk rocksalt and zincblende phases are found to be dynamically unstable, and we show that whereas rocksalt SnS can potentially be stabilized under a reduction of the lattice constant the hypothetical zincblende phase proposed in several previous studies is extremely unlikely to form. We also investigate the stability of Sn2S3 with respect to SnS and SnS2 and find that both dispersion forces and vibrational contributions to the free energy are required to explain its experimentally observed resistance to decomposition.
Date Issued
2017-03-06
Date Acceptance
2017-03-01
Citation
JOURNAL OF PHYSICAL CHEMISTRY C, 2017, 121 (12), pp.6446-6454
ISSN
1932-7447
Publisher
American Chemical Society
Start Page
6446
End Page
6454
Journal / Book Title
JOURNAL OF PHYSICAL CHEMISTRY C
Volume
121
Issue
12
Copyright Statement
© 2017 American Chemical Society. This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Physical Chemistry C after peer review and technical editing by the publisher. To access the final edited and published work see: https://dx.doi.org/10.1021/acs.jpcc.6b12581
Sponsor
The Royal Society
Identifier
http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000398247500004&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202
Grant Number
UF150657
Subjects
Science & Technology
Physical Sciences
Technology
Chemistry, Physical
Nanoscience & Nanotechnology
Materials Science, Multidisciplinary
Chemistry
Science & Technology - Other Topics
Materials Science
AUGMENTED-WAVE METHOD
CUBIC PHASE
SOLAR-CELLS
ZINC BLENDE
THIN-FILMS
SNS
CRYSTAL
SN2S3
DEPOSITION
POLYMORPH
Physical Chemistry
09 Engineering
03 Chemical Sciences
10 Technology
Publication Status
Published