Role of Cation Ordering on Device Performance in (Ag,Cu)InSe2Solar Cells with KF Post-Deposition Treatment

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

Research output: Contribution to journalArticlepeer-review

Abstract

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 (Voc) 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 Voc 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 Voc 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. 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.

Original languageEnglish (US)
Pages (from-to)233-241
Number of pages9
JournalACS Applied Energy Materials
Volume4
Issue number1
DOIs
StatePublished - Jan 25 2021

Keywords

  • Ag alloying
  • Raman spectroscopy
  • Vloss
  • X-ray beam-induced current
  • X-ray fluorescence
  • cation order
  • post-deposition treatment

ASJC Scopus subject areas

  • Chemical Engineering (miscellaneous)
  • Energy Engineering and Power Technology
  • Electrochemistry
  • Materials Chemistry
  • Electrical and Electronic Engineering

Fingerprint Dive into the research topics of 'Role of Cation Ordering on Device Performance in (Ag,Cu)InSe<sub>2</sub>Solar Cells with KF Post-Deposition Treatment'. Together they form a unique fingerprint.

Cite this