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Title: Luminescence of defects in the structural transformation of layered tin dichalcogenides

Abstract

Layered tin sulfide semiconductors are both of fundamental interest and attractive for energy conversion applications. Sn sulfides crystallize in several stable bulk phases with different Sn:S ratios (SnS2, Sn2S3, and SnS), which can transform into phases with a lower sulfur concentration by introduction of sulfur vacancies (VS). How this complex behavior affects the optoelectronic properties remains largely unknown but is of key importance for understanding light-matter interactions in this family of layered materials. In this work, we use the capability to induce VS and drive a transformation between few-layer SnS2 and SnS by electron beam irradiation, combined with in-situ cathodoluminescence spectroscopy and ab-initio calculations to probe the role of defects in the luminescence of these materials. In addition to the characteristic band-edge emission of the endpoint structures, our results show emerging luminescence features accompanying the SnS2 to SnS transformation. Comparison with calculations indicates that the most prominent emission in SnS2 with sulfur vacancies is not due to luminescence from a defect level but involves recombination of excitons bound to neutral VS in SnS2. These results provide insight into the intrinsic and defect-related optoelectronic properties of Sn chalcogenide semiconductors.

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [1]
  1. Univ. of Nebraska, Lincoln, NE (United States)
  2. Aalto Univ., Otaniemi (Finland)
  3. Aalto Univ., Otaniemi (Finland); Helmholtz-Zentrum Dresden-Rossendorf, Dresden (Germany); National Univ. of Science and Technology MISiS, Moscow (Russia)
  4. Chinese Academy of Sciences (CAS), Beijing (China)
Publication Date:
Research Org.:
Univ. of Nebraska, Lincoln, NE (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1527164
Alternate Identifier(s):
OSTI ID: 1414972
Grant/Contract Number:  
SC0016343
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Applied Physics Letters
Additional Journal Information:
Journal Volume: 111; Journal Issue: 26; Journal ID: ISSN 0003-6951
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Sutter, P., Komsa, H. -P., Krasheninnikov, A. V., Huang, Y., and Sutter, E. Luminescence of defects in the structural transformation of layered tin dichalcogenides. United States: N. p., 2017. Web. doi:10.1063/1.5007060.
Sutter, P., Komsa, H. -P., Krasheninnikov, A. V., Huang, Y., & Sutter, E. Luminescence of defects in the structural transformation of layered tin dichalcogenides. United States. https://doi.org/10.1063/1.5007060
Sutter, P., Komsa, H. -P., Krasheninnikov, A. V., Huang, Y., and Sutter, E. 2017. "Luminescence of defects in the structural transformation of layered tin dichalcogenides". United States. https://doi.org/10.1063/1.5007060. https://www.osti.gov/servlets/purl/1527164.
@article{osti_1527164,
title = {Luminescence of defects in the structural transformation of layered tin dichalcogenides},
author = {Sutter, P. and Komsa, H. -P. and Krasheninnikov, A. V. and Huang, Y. and Sutter, E.},
abstractNote = {Layered tin sulfide semiconductors are both of fundamental interest and attractive for energy conversion applications. Sn sulfides crystallize in several stable bulk phases with different Sn:S ratios (SnS2, Sn2S3, and SnS), which can transform into phases with a lower sulfur concentration by introduction of sulfur vacancies (VS). How this complex behavior affects the optoelectronic properties remains largely unknown but is of key importance for understanding light-matter interactions in this family of layered materials. In this work, we use the capability to induce VS and drive a transformation between few-layer SnS2 and SnS by electron beam irradiation, combined with in-situ cathodoluminescence spectroscopy and ab-initio calculations to probe the role of defects in the luminescence of these materials. In addition to the characteristic band-edge emission of the endpoint structures, our results show emerging luminescence features accompanying the SnS2 to SnS transformation. Comparison with calculations indicates that the most prominent emission in SnS2 with sulfur vacancies is not due to luminescence from a defect level but involves recombination of excitons bound to neutral VS in SnS2. These results provide insight into the intrinsic and defect-related optoelectronic properties of Sn chalcogenide semiconductors.},
doi = {10.1063/1.5007060},
url = {https://www.osti.gov/biblio/1527164}, journal = {Applied Physics Letters},
issn = {0003-6951},
number = 26,
volume = 111,
place = {United States},
year = {Wed Dec 27 00:00:00 EST 2017},
month = {Wed Dec 27 00:00:00 EST 2017}
}

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Cited by: 15 works
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Figures / Tables:

FIG. 1 FIG. 1: Electron-beam induced transformation of few-layer SnS2 to SnS at elevated temperatures. (a) TEM image of SnS2 flakes at 100°C at the initial stages of the electron-beam induced transformation. (b) Electron diffraction pattern showing pure trigonal SnS2 along the [001] zone axis (ZA, equivalent to [0001] in Bravais-Miller 4more » index notation). Similarly, the (010) plane is identical to the ($$01\bar1 0$$) plane and the (110) plane to the ($$11\bar2 0$$) plane. (c) HRTEM lattice image of the starting material, showing the characteristic 6-fold symmetry of layered SnS2. 1 (d) TEM image of the same region shown in (a) after exposure to the electron beam at 400°C, which causes a transformation to uniform SnS over large areas along with an overall loss of material. (e) Electron diffraction pattern showing the pure orthorhombic a-SnS crystal structure along the [011] ZA. (d) HRTEM lattice image of the transformed flake, showing the orthorhombic structure of few-layer SnS.« less

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Works referencing / citing this record:

Van der Waals SnSe 2(1− x ) S 2 x Alloys: Composition‐Dependent Bowing Coefficient and Electron–Phonon Interaction
journal, December 2019


Wrap‐Around Core–Shell Heterostructures of Layered Crystals
journal, May 2019


Direct optical-structure correlation in atomically thin dichalcogenides and heterostructures
journal, January 2020


Exploring single-layered SnSe honeycomb polymorphs for optoelectronic and photovoltaic applications
journal, February 2018


Direct optical-structure correlation in atomically thin dichalcogenides and heterostructures
journal, January 2020


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