Modification of defects and potential fluctuations in slow-cooled and quenched Cu2ZnSnSe4 single crystals

Bishop, Douglas M.; McCandless, Brian; Gershon, Talia; Lloyd, Michael A.; Haight, Richard; Birkmire, Robert

doi:10.1063/1.4975483

Title: Modification of defects and potential fluctuations in slow-cooled and quenched Cu₂ZnSnSe₄ single crystals

Journal Article · Mon Feb 13 00:00:00 EST 2017 · Journal of Applied Physics

DOI:https://doi.org/10.1063/1.4975483· OSTI ID:1465326

^[1]; McCandless, Brian ^[2]; Gershon, Talia ^[3]; Lloyd, Michael A. ^[2]; Haight, Richard ^[3];

^[2]

Univ. of Delaware, Newark, DE (United States). Inst. of Energy Conversion; IBM T. J. Watson Research Center, Yorktown Heights, NY (United States)
Univ. of Delaware, Newark, DE (United States). Inst. of Energy Conversion
IBM T. J. Watson Research Center, Yorktown Heights, NY (United States)

Recent literature reports have shown the ability to manipulate Cu-Zn cation ordering for Cu₂ZnSnSe₄ (CZTSe) via low temperature treatments. Theoretical arguments suggest that one of the major roadblocks to higher V_OC—significant band tailing—could be improved with increased cation order; however, few direct measurements have been reported and significant device improvements have not yet been realized. This paper investigates electrical properties, defects, and devices from quenched and slow-cooled single crystals of CZTSe. The extent of disorder was characterized by Raman spectroscopy as well as x-ray diffraction, where the change in Cu-Zn order can be detected by a changing c/a ratio. Quenched samples show higher acceptor concentrations, lower hole mobilities, and a lower-energy photoluminescence (PL) peak than crystals cooled at slower rates, consistent with a reduction in the bandgap. In addition, samples quenched at the highest temperatures showed lower PL yield consistent with higher quantities of deep defects. Devices fabricated using slow-cooled CZTSe single crystals showed improved efficiencies, most notably with increased V_OC; however, low temperature intensity-dependent photoluminescence measurements continue to indicate the existence of potential fluctuations. We discuss the possibility that potential fluctuations in slow-cooled samples may be related to the inability to achieve a long range order of the Cu-Zn sub-lattice resulting in local regions of high and low levels of cation order, and consequent local variations in the bandgap. Finally, the presence of significant potential fluctuations, even after the slow-cooling step, suggests the difficulty in eliminating band-tailing in this system, and thus, additional approaches may be needed for significant reduction of the V_OC deficit.

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Research Organization:: IBM T. J. Watson Research Center, Yorktown Heights, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office

Grant/Contract Number:: EE0006334

OSTI ID:: 1465326

Alternate ID(s):: OSTI ID: 1361769

Journal Information:: Journal of Applied Physics, Vol. 121, Issue 6; ISSN 0021-8979

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 16 works

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Cited By (2)

Majority Carrier Properties of Single Crystal Cu 2− x ZnSnSe 4 with Varying Copper Composition McCandless, Brian E.; Bishop, Doug; Lloyd, Michael physica status solidi (b), Vol. 256, Issue 11 https://doi.org/10.1002/pssb.201900180	journal	July 2019
The effect of stoichiometry on Cu-Zn ordering kinetics in Cu ₂ ZnSnS ₄ thin films Rudisch, Katharina; Davydova, Alexandra; Platzer-Björkman, Charlotte Journal of Applied Physics, Vol. 123, Issue 16 https://doi.org/10.1063/1.5010081	journal	April 2018

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Title: Modification of defects and potential fluctuations in slow-cooled and quenched Cu2ZnSnSe4 single crystals

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Title: Modification of defects and potential fluctuations in slow-cooled and quenched Cu₂ZnSnSe₄ single crystals