Crystal reconstruction and defect healing enabled high-quality SbSe films for solar cell applications

Sb 2 Se 3 is a kind of quasi-one-dimensional solar cell absorber material, the crystal orientation and deep-level defects sensitively affect the energy conversion in Sb 2 Se 3 solar cells. Conventionally, the development of the film synthesis method to control the crystallinity as well as the defects has been well studied, while the current methods show limited capability in tuning the critical parameters. Here, we develop a novel post-sulfurization method to manipulate the crystallization of Sb 2 Se 3 films, which yields excellent grain structures and provides effective defect passivation. This method treats the thermal evaporation deposited Sb 2 Se 3 layer using an innovative sulfurization configuration. We find that the crystals of the Sb 2 Se 3 films are reconstructed by post-treatment with sulfur gas, yielding high-quality Sb 2 Se 3 with benign [ hkl ] growth orientation, a smooth surface, and large compact crystal grains. Moreover, this engineering strategy remarkably mitigates the device open-circuit voltage deficit because of the effectively healed deep level defects. As a result, photovoltaic devices subjected to this post-treatment exhibit markedly improved performance compared to controlled solar cells. This study demonstrates a new sulfurization approach for optimizing the crystallinity and deep-level defects and overall efficiency of Sb 2 Se 3 solar cells. A post-sulfurization technique has been developed to refine Sb 2 Se 3 crystallization. This process enables high-quality Sb 2 Se 3 with a smooth surface, large compact crystal grains and benign [ hkl ] growth orientation. It also mitigates the device V OC deficit, owing to the healed deep level defects.