Role of Cation Ordering on Device Performance in (Ag,Cu)InSe2 Solar Cells with KF Post-Deposition Treatment

Nietzold, Tara; Valdes, Nicholas; Stuckelberger, Michael E.; Chui, Michelle; Walker, Trumann; Jeffries, April M.; Sinha, Archana; Schelhas, Laura T.; Lai, Barry; Shafarman, William N.; Bertoni, Mariana I.

doi:10.1021/acsaem.0c02197

Title: Role of Cation Ordering on Device Performance in (Ag,Cu)InSe₂ Solar Cells with KF Post-Deposition Treatment

Journal Article · Mon Jan 11 00:00:00 UTC 2021 · ACS Applied Energy Materials

DOI: https://doi.org/10.1021/acsaem.0c02197 · OSTI ID:1756715

^[1];

^[2];

^[3]; Chui, Michelle ^[4];

^[4]; Jeffries, April M. ^[4];

^[5];

^[5]; Lai, Barry ^[6]; Shafarman, William N. ^[2];

^[4]

Arizona State Univ., Tempe, AZ (United States); Arizona State University
Univ. of Delaware, Newark, DE (United States)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
Arizona State Univ., Tempe, AZ (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Argonne National Lab. (ANL), Lemont, IL (United States). Advanced Photon Source (APS)

CuInSe₂(CIS) has been proposed as an attractive bottom cell candidate in tandem solar cells. However, to justify the coupling with high-performance top cells (e.g., perovskites, GaAs), significant work on improving the efficiency is required. To this extent, several authors have demonstrated the benefits of alkali post-deposition treatments (PDT) to increase device open-circuit voltage (V_oc) in CIS and how Ag alloying - (Ag,Cu)InSe₂(ACIS) - reduces defect density and enhances current collection in devices. Herein, we present a detailed study of the role that KF-PDT plays on CIS and ACIS absorber composition and structure, and propose an explanation for the decreased V_oc observed when silver and potassium coexist in the system (ACIS + KF). Through a suite of synchrotron-based techniques, we investigate the nanoscale chemical distribution of the films and the formation of secondary phases. Through photoluminescence imaging, we observed a high degree of passivation with the addition of KF, and synchrotron-based X-ray diffraction confirmed the absence of a KInSe₂ surface layer usually considered to be a passivating agent. Raman spectroscopy and synchrotron X-ray fluorescence show the increased presence of Cu- and Se-poor clusters in ACIS + KF, which are correlated to significantly reduced X-ray beam-induced current (XBIC). An increase in the intensity of the E/B₂ stretching mode of CIS is attributed to cation ordering near the junction and is found to track inversely to bulk V_oc measurements. The cation ordering is hypothesized to arise from the formation and redistribution of defects that normally occur near the surfaces of CIS as a consequence of its polar character. Here, these defects compensate each other, and the overall inhomogeneity of the charge distribution generates electrostatic potential fluctuations that greatly increase the saturation current and hence reduce the open-circuit voltage of the device.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Arizona State Univ., Tempe, AZ (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); SLAC National Accelerator Laboratory, Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)

Sponsoring Organization:: Engineering Research Center QESST; National Science Foundation (NSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; AC02-76SF00515; EE0008163

OSTI ID:: 1756715

Journal Information:: ACS Applied Energy Materials, Journal Name: ACS Applied Energy Materials Journal Issue: 1 Vol. 4; ISSN 2574-0962

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Ag-alloying
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V oc loss
Voc loss
X-ray beam induced current
X-ray fluorescence
cation order
post-deposition treatment

Title: Role of Cation Ordering on Device Performance in (Ag,Cu)InSe2 Solar Cells with KF Post-Deposition Treatment

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Title: Role of Cation Ordering on Device Performance in (Ag,Cu)InSe₂ Solar Cells with KF Post-Deposition Treatment