Laser-Annealing and Solid-Phase Epitaxy of Selenium Thin-Film Solar Cells

Selenium has resurged as a promising photovoltaic material in solar cell research due to its wide direct bandgap of 1.95 eV, making it a suitable candidate for a top cell in tandem photovoltaic devices. However, the optoelectronic quality of selenium thin-films has been identified as a key bottleneck for realizing high-efficiency selenium solar cells. In this study, we present an approach for crystallizing selenium thin-films using laser-annealing as an alternative to the conventionally used thermal annealing strategy. By laser-annealing through a semitransparent substrate, a buried layer of high-quality selenium crystallites is formed and used as a growth template for solid-phase epitaxy. The resulting selenium thin-films feature larger and more preferentially oriented grains with a negligible surface roughness in comparison to thermally annealed selenium thin-films. We fabricate photovoltaic devices using this strategy and demonstrate a record ideality factor of n = 1.37, a record fill factor of FF = 63.7%, and a power conversion efficiency of PCE = 5.0%. The presented laser-annealing strategy is universally applicable and is a promising approach for crystallizing a wide range of photovoltaic materials where high temperatures are needed while maintaining a low substrate temperature.