<p>Sb<sub>2</sub>Se<sub>3 </sub>has emerged as an important photoelectrochemical (PEC) and photovoltaic (PV) material due to its rapid rise in photoconversion efficiencies. However, despite its binary nature, Sb<sub>2</sub>Se<sub>3 </sub>has a complex defect chemistry, which reduces the maximum photovoltage that can be obtained. Thus, it is important to understand these defects and to develop passivation strategies in order to further improve this material. In this work, a comprehensive investigation of the charge carrier dynamics of Sb<sub>2</sub>Se<sub>3</sub> and the influence of sulfur treatment on its optoelectronic properties was performed using time resolved microwave conductivity (TRMC), photoluminescence (PL) spectroscopy and low frequency Raman spectroscopy (LFRS). The key finding in this work is that upon sulfur treatment of Sb<sub>2</sub>Se<sub>3</sub>, the carrier lifetime is increased by the passivation of deep defects in Sb<sub>2</sub>Se<sub>3</sub> in both the surface region and the bulk, which is evidenced by increased charge carrier lifetime of TRMC decay dynamics, increased radiative recombination efficiency and decreased deep defect level emission (PL), and improved long-range order in the material (LFRS). These findings provide crucial insights into the defect passivation mechanisms in Sb<sub>2</sub>Se<sub>3</sub> paving the way for developing highly efficient PEC and PV devices.</p>
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