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Title: Point defects in Cu 2 ZnSnSe 4 (CZTSe): Resonant X-ray diffraction study of the low-temperature order/disorder transition: Point defects in Cu 2 ZnSnSe 4 (CZTSe)

Abstract

The interest in Cu2ZnSn(S,Se)4 (CZTS) for photovoltaic applications is motivated by similarities to Cu(In,Ga)Se2 while being comprised of non-toxic and earth abundant elements. However, CZTS suffers from a Voc deficit, where the Voc is much lower than expected based on the band gap, which may be the result of a high concentration of point-defects in the CZTS lattice. Recently, reports have observed a low-temperature order/disorder transition by Raman and optical spectroscopies in CZTS films and is reported to describe the ordering of Cu and Zn atoms in the CZTS crystal structure. To directly determine the level of Cu/Zn ordering, we have used resonant-XRD, a site, and element specific probe of long range order. We used CZTSe films annealed just below and quenched from just above the transition temperature; based on previous work, the Cu and Zn should be ordered and highly disordered, respectively. Our data show that there is some Cu/Zn ordering near the low temperature transition but significantly less than high chemical order expected from Raman. To understand both our resonant-XRD results and the Raman results, we present a structural model that involves antiphase domain boundaries and accommodates the excess Zn within the CZTS lattice.

Authors:
 [1];  [2];  [3];  [4];  [4];  [3];  [3];  [5]
  1. Applied Energy Programs, SLAC National Accelerator Laboratory, Menlo Park California 94025 USA
  2. Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park California 94025 USA
  3. National Renewable Energy Laboratory, Golden Colorado 80401 USA
  4. Materials Science and Engineering Department, Stanford University, Stanford CA 94305 USA
  5. Applied Energy Programs, SLAC National Accelerator Laboratory, Menlo Park California 94025 USA; Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park California 94025 USA
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1398877
Report Number(s):
NREL/JA-5K00-70251
Journal ID: ISSN 0370-1972
DOE Contract Number:  
AC36-08GO28308
Resource Type:
Journal Article
Journal Name:
Physica Status Solidi B. Basic Solid State Physics
Additional Journal Information:
Journal Volume: 254; Journal Issue: 9; Journal ID: ISSN 0370-1972
Publisher:
Wiley-Blackwell
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; Cu2ZnSnSe; order-disorder transitions; point defects; thin films; X-ray diffraction

Citation Formats

Schelhas, L. T., Stone, K. H., Harvey, S. P., Zakhidov, D., Salleo, A., Teeter, G., Repins, I. L., and Toney, M. F. Point defects in Cu 2 ZnSnSe 4 (CZTSe): Resonant X-ray diffraction study of the low-temperature order/disorder transition: Point defects in Cu 2 ZnSnSe 4 (CZTSe). United States: N. p., 2017. Web. doi:10.1002/pssb.201700156.
Schelhas, L. T., Stone, K. H., Harvey, S. P., Zakhidov, D., Salleo, A., Teeter, G., Repins, I. L., & Toney, M. F. Point defects in Cu 2 ZnSnSe 4 (CZTSe): Resonant X-ray diffraction study of the low-temperature order/disorder transition: Point defects in Cu 2 ZnSnSe 4 (CZTSe). United States. doi:10.1002/pssb.201700156.
Schelhas, L. T., Stone, K. H., Harvey, S. P., Zakhidov, D., Salleo, A., Teeter, G., Repins, I. L., and Toney, M. F. Tue . "Point defects in Cu 2 ZnSnSe 4 (CZTSe): Resonant X-ray diffraction study of the low-temperature order/disorder transition: Point defects in Cu 2 ZnSnSe 4 (CZTSe)". United States. doi:10.1002/pssb.201700156.
@article{osti_1398877,
title = {Point defects in Cu 2 ZnSnSe 4 (CZTSe): Resonant X-ray diffraction study of the low-temperature order/disorder transition: Point defects in Cu 2 ZnSnSe 4 (CZTSe)},
author = {Schelhas, L. T. and Stone, K. H. and Harvey, S. P. and Zakhidov, D. and Salleo, A. and Teeter, G. and Repins, I. L. and Toney, M. F.},
abstractNote = {The interest in Cu2ZnSn(S,Se)4 (CZTS) for photovoltaic applications is motivated by similarities to Cu(In,Ga)Se2 while being comprised of non-toxic and earth abundant elements. However, CZTS suffers from a Voc deficit, where the Voc is much lower than expected based on the band gap, which may be the result of a high concentration of point-defects in the CZTS lattice. Recently, reports have observed a low-temperature order/disorder transition by Raman and optical spectroscopies in CZTS films and is reported to describe the ordering of Cu and Zn atoms in the CZTS crystal structure. To directly determine the level of Cu/Zn ordering, we have used resonant-XRD, a site, and element specific probe of long range order. We used CZTSe films annealed just below and quenched from just above the transition temperature; based on previous work, the Cu and Zn should be ordered and highly disordered, respectively. Our data show that there is some Cu/Zn ordering near the low temperature transition but significantly less than high chemical order expected from Raman. To understand both our resonant-XRD results and the Raman results, we present a structural model that involves antiphase domain boundaries and accommodates the excess Zn within the CZTS lattice.},
doi = {10.1002/pssb.201700156},
journal = {Physica Status Solidi B. Basic Solid State Physics},
issn = {0370-1972},
number = 9,
volume = 254,
place = {United States},
year = {2017},
month = {7}
}

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