Lattice dynamics of the tin sulphides SnS2, SnS and Sn2S3: vibrational spectra and thermal transport
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Published version
Author(s)
Type
Journal Article
Abstract
We present an in-depth first-principles study of the lattice dynamics of the tin sulphides SnS2, Pnma and π-cubic SnS and Sn2S3. An analysis of the harmonic phonon dispersion and vibrational density of states reveals phonon bandgaps between low- and high-frequency modes consisting of Sn and S motion, respectively, and evidences a bond-strength hierarchy in the low-dimensional SnS2, Pnma SnS and Sn2S3 crystals. We model and perform a complete characterisation of the infrared and Raman spectra, including temperature-dependent anharmonic linewidths calculated using many-body perturbation theory. We illustrate how vibrational spectroscopy could be used to identify and characterise phase impurities in tin sulphide samples. The spectral linewidths are used to model the thermal transport, and the calculations indicate that the low-dimensional Sn2S3 has a very low lattice thermal conductivity, potentially giving it superior performance to SnS as a candidate thermoelectric material.
Date Issued
2017-05-03
Date Acceptance
2017-04-27
Citation
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2017, 19 (19), pp.12452-12465
ISSN
1463-9076
Publisher
Royal Society of Chemistry
Start Page
12452
End Page
12465
Journal / Book Title
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume
19
Issue
19
Copyright Statement
© 2017 the Owner Societies. Open Access. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence (https://creativecommons.org/licenses/by/3.0/).
Sponsor
The Royal Society
Identifier
http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000401640600073&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202
Grant Number
UF150657
Subjects
Science & Technology
Physical Sciences
Chemistry, Physical
Physics, Atomic, Molecular & Chemical
Chemistry
Physics
CHEMICAL-VAPOR-DEPOSITION
AUGMENTED-WAVE METHOD
FILM SOLAR-CELLS
THIN-FILMS
HIGH-TEMPERATURE
THERMOELECTRIC-MATERIALS
HIGH-PRESSURE
CUBIC PHASE
ZINC BLENDE
CRYSTAL
Chemical Physics
02 Physical Sciences
03 Chemical Sciences
Publication Status
Published