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Mapping the Energetics of Defect States in Cu2ZnSnS4 films and the Impact of Sb Doping.

Authors
  • Tiwari, Devendra1, 2
  • Yakushev, Michael V3, 4, 5, 6
  • Koehler, Tristan7
  • Cattelan, Mattia2
  • Fox, Neil2, 8
  • Martin, Robert W3
  • Klenk, Reiner9
  • Férmin, David J2
  • 1 Department of Mathematics, Physics and Electrical Engineering, Northumbria University, Ellison Place, NE1 8ST Newcastle upon Tyne, United Kingdom. , (United Kingdom)
  • 2 School of Chemistry, University of Bristol, Cantocks Close, BS8 1TS Bristol, United Kingdom. , (United Kingdom)
  • 3 Department of Physics, SUPA, Strathclyde University, G4 0NG Glasgow, United Kingdom. , (United Kingdom)
  • 4 M.N. Miheev Institute of Metal Physics of the UB RAS, 18 S. Kovalevskoy St., 620108 Ekaterinburg, Russia.
  • 5 Ural Federal University, 19 Mira St., 620002 Ekaterinburg, Russia.
  • 6 Institute of Solid-State Chemistry of the UB RAS, 620990 Ekaterinburg, Russia.
  • 7 Faculty of Physics, University of Duisburg-Essen, Forsthausweg 2, 47057 Duisburg, Germany. , (Germany)
  • 8 H. H. Wills Physics Laboratory, University of Bristol, Tyndall Avenue, BS8 1TL Bristol, United Kingdom. , (United Kingdom)
  • 9 Helmholtz-Zentrum Berlin für Materialien und Energie, Hahn-Meitner-Platz 1, D-14109 Berlin, Germany. , (Germany)
Type
Published Article
Journal
ACS Applied Energy Materials
Publisher
American Chemical Society (ACS)
Publication Date
Apr 25, 2022
Volume
5
Issue
4
Pages
3933–3940
Identifiers
DOI: 10.1021/acsaem.1c03729
PMID: 35497685
Source
Medline
Language
English
License
Unknown

Abstract

The sub-bandgap levels associated with defect states in Cu2ZnSnS4 (CZTS) thin films are investigated by correlating the temperature dependence of the absorber photoluminescence (PL) with the device admittance spectroscopy. CZTS thin films are prepared by thermolysis of molecular precursors incorporating chloride salts of the cations and thiourea. Na and Sb are introduced as dopants in the precursor layers to assess their impact on Cu/Zn and Sn site disorder, respectively. Systematic analysis of PL spectra as a function of excitation power and temperature show that radiative recombination is dominated by quasi-donor-acceptor pairs (QDAP) with a maximum between 1.03 and 1.18 eV. It is noteworthy that Sb doping leads to a transition from localized to delocalized QDAP. The activation energies obtained associated with QDAP emission closely correlate with the activation energies of the admittance responses in a temperature range between 150 K and room temperature in films with or without added dopants. Admittance data of CZTS films with no added dopants also have a strong contribution from a deeper state associated with Sn disorder. The ensemble of PL and admittance data, in addition to energy-filtered photoemission of electron microscopy (EF-PEEM), shows a detailed picture of the distribution of sub-bandgap states in CZTS and the impact of doping on their energetics and device performance. © 2022 The Authors. Published by American Chemical Society.

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