Phase stability of the earth-abundant tin sulfides SnS, SnS2, and Sn2S3
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Published version
Author(s)
Burton, LA
Walsh, A
Type
Journal Article
Abstract
The various phases of tin sulfide have been studied as semiconductors since the 1960s and are now being investigated as potential earth-abundant photovoltaic and photocatalytic materials. Of particular note is the recent isolation of zincblende SnS in particles and thin-films. Herein, first-principles calculations are employed to better understand this novel geometry and its place within the tin sulfide multiphasic system. We report the enthalpies of formation for the known phases of SnS, SnS2, and Sn2S3, with good agreement between theory and experiment for the ground-state structures of each. While theoretical X-ray diffraction patterns do agree with the assignment of the zincblende phase demonstrated in the literature, the structure is not stable close to the lattice parameters observed experimentally, exhibiting an unfeasibly large pressure and a formation enthalpy much higher than any other phase. Ab initio molecular dynamics simulations reveal spontaneous degradation to an amorphous phase much lower in energy, as Sn(II) is inherently unstable in a regular tetrahedral environment. We conclude that the known rocksalt phase of SnS has been mis-assigned as zincblende in the recent literature.
Date Issued
2012-11-15
Date Acceptance
2012-10-24
Citation
Journal of Physical Chemistry C, 2012, 116 (45), pp.24262-24267
ISSN
1932-7455
Publisher
American Chemical Society
Start Page
24262
End Page
24267
Journal / Book Title
Journal of Physical Chemistry C
Volume
116
Issue
45
Copyright Statement
© 2012 American Chemical Society. his is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes. (http://pubs.acs.org/page/policy/authorchoice_termsofuse.html)
Identifier
http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000311190800052&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202
Subjects
Science & Technology
Physical Sciences
Technology
Chemistry, Physical
Nanoscience & Nanotechnology
Materials Science, Multidisciplinary
Chemistry
Science & Technology - Other Topics
Materials Science
Film solar-cells
Thin-films
Optical-properties
Single-crystals
Zinc blende
Deposition
Efficiency
Pressure
Monochalcogenides
Electrodeposition
Physical Chemistry
Engineering
Chemical Sciences
10 Technology
Publication Status
Published