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:https://doi.org/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

Bar-Ilan University

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

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

Keywords

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

All Science Journal Classification (ASJC) codes

Electronic, Optical and Magnetic Materials
General Chemistry
Condensed Matter Physics
General Materials Science
Electrochemistry
Biomaterials

UN SDGs

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

Access to Document

https://doi.org/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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title = "Sulfur Treatment Passivates Bulk Defects in Sb2Se3 Photocathodes for Water Splitting",

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.",

keywords = "Sb Se, charge carrier dynamics, low-frequency Raman spectroscopy, photoluminescence spectroscopy, time-resolved microwave conductivity",

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

note = "Publisher Copyright: {\textcopyright} 2022 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH.",

year = "2022",

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T1 - Sulfur Treatment Passivates Bulk Defects in Sb2Se3 Photocathodes for Water Splitting

AU - Prabhakar, Rajiv Ramanujam

AU - Moehl, Thomas

AU - Friedrich, Dennis

AU - Kunst, Marinus

AU - Shukla, Sudhanshu

AU - Adeleye, Damilola

AU - Damle, Vinayaka H.

AU - Siol, Sebastian

AU - Cui, Wei

AU - Gouda, Laxman

AU - Suh, Jihye

AU - Tischler, Yaakov R.

AU - van de Krol, Roel

AU - Tilley, S. David

PY - 2022/6/17

Y1 - 2022/6/17

N2 - 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.

AB - 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.

KW - Sb Se

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KW - low-frequency Raman spectroscopy

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