Sulfur Treatment Passivates Bulk Defects in Sb2Se3 Photocathodes for Water Splitting

Rajiv Ramanujam Prabhakar; Thomas Moehl; Dennis Friedrich; Marinus Kunst; Sudhanshu Shukla; Damilola Adeleye; Vinayaka H. Damle; Sebastian Siol; Wei Cui; Laxman Gouda; Jihye Suh; Yaakov R. Tischler; Roel van de Krol; S. David Tilley

doi:10.1002/adfm.202112184

Sulfur Treatment Passivates Bulk Defects in Sb₂Se₃ Photocathodes for Water Splitting

Rajiv Ramanujam Prabhakar
, Thomas Moehl
, Dennis Friedrich
, Marinus Kunst
, Sudhanshu Shukla
, Damilola Adeleye
, Vinayaka H. Damle
, Sebastian Siol
, Wei Cui
, Laxman Gouda
, Jihye Suh
, Yaakov R. Tischler
, Roel van de Krol
, S. David Tilley

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

28 Scopus citations

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.

Original language	English
Article number	2112184
Journal	Advanced Functional Materials
Volume	32
Issue number	25
DOIs	https://doi.org/10.1002/adfm.202112184
State	Published - 17 Jun 2022

Bibliographical note

Publisher Copyright:
© 2022 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH.

Funding

S.D.T. thanks the Swiss National Science Foundation (AP Energy Grant PYAPP2 160586) and the University Research Priority Program LightChEC for funding. S.S. acknowledges funding from Luxembourgish Fond National de la Recherche FNR through the MASSENA project. Y.R.T. acknowledges Israel Ministry of Science and Technology (MOST) Optoelectronics grant (grant number 205509) for funding. S.D.T. thanks the Swiss National Science Foundation (AP Energy Grant PYAPP2 160586) and the University Research Priority Program LightChEC for funding. S.S. acknowledges funding from Luxembourgish Fond National de la Recherche FNR through the MASSENA project. Y.R.T. acknowledges Israel Ministry of Science and Technology (MOST) Optoelectronics grant (grant number 205509) for funding. Open access funding provided by Universitat Zurich.

Funders	Funder number
Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung	PYAPP2 160586
Fonds National de la Recherche Luxembourg
Ministry of Science and Technology, Taiwan	205509
Ministry of science and technology, Israel
Universität Zürich

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Keywords

Sb Se
charge carrier dynamics
low-frequency Raman spectroscopy
photoluminescence spectroscopy
time-resolved microwave conductivity

Access to Document

10.1002/adfm.202112184

Cite this

Prabhakar, R. R., Moehl, T., Friedrich, D., Kunst, M., Shukla, S., Adeleye, D., Damle, V. H., Siol, S., Cui, W., Gouda, L., Suh, J., Tischler, Y. R., van de Krol, R., & Tilley, S. D. (2022). Sulfur Treatment Passivates Bulk Defects in Sb₂Se₃ Photocathodes for Water Splitting. Advanced Functional Materials, 32(25), Article 2112184. https://doi.org/10.1002/adfm.202112184

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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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AU - Shukla, Sudhanshu

AU - Adeleye, Damilola

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AU - Siol, Sebastian

AU - Cui, Wei

AU - Gouda, Laxman

AU - Suh, Jihye

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