Abstract

Hydrothermal deposition is emerging as a highly potential route for antimony-based solar cells, in which the Sb2(S,Se)3 is typically in situ grown on a common toxic CdS buffer layer. The narrow band gap of CdS causes a considerable absorption in the short-wavelength region and then lowers the current density of the device. Herein, TiO2 is first evaluated as an alternative Cd-free buffer layer for hydrothermally derived Sb2S3 solar cells. But it suffers from a severely inhomogeneous Sb2S3 coverage, which is effectively eliminated by inserting a Zn(O,S) layer. The surface atom of sulfur in Zn(O,S) uniquely provides a chemical bridge to enable the quasi-epitaxial deposition of Sb2S3 thin film, confirming by both morphology and binding energy analysis using DFT. Then the results of the first-principles calculations also show that Zn(O,S)/Sb2S3 has a more stable structure than TiO2/Sb2S3. The resultant perfect Zn(O,S)/Sb2S3 junction, with a suitable band alignment and excellent interface contact, delivers a remarkably enhanced JSC and VOC for Sb2S3 solar cells. The device efficiency with the TiO2/Zn(O,S) buffer layer boosts from 0.54% to 3.70% compared with the counterpart of TiO2, which has a champion efficiency of Cd-free Sb2S3 solar cells with a structure of ITO/TiO2/Zn(O,S)/Sb2S3/Carbon/Ag by in situ hydrothermal deposition. This work provides a guideline for the hydrothermal deposition of antimony-based films upon a nontoxic buffer layer.

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