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Sulfur-Treatment Passivates Bulk Defects in Sb2Se3 Photocathodes for Water Splitting


Prabhakar, Rajiv Ramanujam; Moehl, Thomas; Friedrich, Dennis; Kunst, Marinus; Shukla, Sudhanshu; Adeleye, Damilola; Damle, Vinayaka H; Siol, Sebastian; Cui, Wei; Gouda, Laxman; Suh, Jihye; Tischler, Yaakov R; van de Krol, Roel; Tilley, S David (2022). Sulfur-Treatment Passivates Bulk Defects in Sb2Se3 Photocathodes for Water Splitting. Advanced Functional Materials, 32(25):2112184.

Abstract

Sb2Se3 has emerged as an important photoelectrochemical (PEC) and photovoltaic (PV) material due to its rapid rise in photoconversion efficiencies. However, Sb2Se3 has a complex defect chemistry, which reduces the maximum photovoltage. Thus, it is important to understand these defects and develop defect passivation strategies in Sb2Se3. A comprehensive investigation of the charge carrier dynamics of Sb2Se3 and the influence of sulfur treatment on its optoelectronic properties is performed using time-resolved microwave conductivity (TRMC), photoluminescence (PL) spectroscopy, and low-frequency Raman spectroscopy (LFR). The key finding in this work is that upon sulfur treatment of Sb2Se3, the carrier lifetime is increased by the passivation of deep defects in Sb2Se3 in both the surface region and the bulk, which is evidenced by increased charge carrier lifetime of TRMC decay dynamics, increased radiative recombination efficiency, decreased deep defect level emission (PL), and the emergence of new vibration modes by LFR.

Abstract

Sb2Se3 has emerged as an important photoelectrochemical (PEC) and photovoltaic (PV) material due to its rapid rise in photoconversion efficiencies. However, Sb2Se3 has a complex defect chemistry, which reduces the maximum photovoltage. Thus, it is important to understand these defects and develop defect passivation strategies in Sb2Se3. A comprehensive investigation of the charge carrier dynamics of Sb2Se3 and the influence of sulfur treatment on its optoelectronic properties is performed using time-resolved microwave conductivity (TRMC), photoluminescence (PL) spectroscopy, and low-frequency Raman spectroscopy (LFR). The key finding in this work is that upon sulfur treatment of Sb2Se3, the carrier lifetime is increased by the passivation of deep defects in Sb2Se3 in both the surface region and the bulk, which is evidenced by increased charge carrier lifetime of TRMC decay dynamics, increased radiative recombination efficiency, decreased deep defect level emission (PL), and the emergence of new vibration modes by LFR.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
08 Research Priority Programs > Solar Light to Chemical Energy Conversion
Dewey Decimal Classification:540 Chemistry
Scopus Subject Areas:Physical Sciences > General Chemistry
Physical Sciences > General Materials Science
Physical Sciences > Condensed Matter Physics
Uncontrolled Keywords:Electrochemistry, Condensed Matter Physics, Biomaterials, Electronic, Optical and Magnetic Materials
Language:English
Date:1 June 2022
Deposited On:24 Mar 2022 07:46
Last Modified:28 Jan 2024 02:46
Publisher:Wiley-Blackwell Publishing, Inc.
ISSN:1616-301X
OA Status:Hybrid
Free access at:Publisher DOI. An embargo period may apply.
Publisher DOI:https://doi.org/10.1002/adfm.202112184
Project Information:
  • : FunderSNSF
  • : Grant IDPYAPP2_160586
  • : Project TitleSolar Water Splitting: Photovoltage, Surface Dipole, and Catalysis Strategies
  • Content: Published Version
  • Licence: Creative Commons: Attribution 4.0 International (CC BY 4.0)