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)

Schelhas, L. T.; Stone, K. H.; Harvey, S. P.; Zakhidov, D.; Salleo, A.; Teeter, G.; Repins, I. L.; Toney, M. F.

doi:10.1002/pssb.201700156

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)

Journal Article · Tue Jul 25 00:00:00 EDT 2017 · Physica Status Solidi B. Basic Solid State Physics

DOI:https://doi.org/10.1002/pssb.201700156· OSTI ID:1398877

Schelhas, L. T. ^[1]; Stone, K. H. ^[2]; Harvey, S. P. ^[3]; Zakhidov, D. ^[4]; Salleo, A. ^[4]; Teeter, G. ^[3]; Repins, I. L. ^[3]; Toney, M. F. ^[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
National Renewable Energy Laboratory, Golden Colorado 80401 USA
Materials Science and Engineering Department, Stanford University, Stanford CA 94305 USA
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

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.

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Research Organization:: National Renewable Energy Lab. (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

DOE Contract Number:: AC36-08GO28308

OSTI ID:: 1398877

Report Number(s):: NREL/JA-5K00-70251

Journal Information:: Physica Status Solidi B. Basic Solid State Physics, Vol. 254, Issue 9; ISSN 0370-1972

Publisher:: Wiley-Blackwell

Country of Publication:: United States

Language:: English

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