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Selenium has resurged as a promising photovoltaic material in solar cellresearch due to its wide direct bandgap of 1.95 eV, making it a suitablecandidate for a top cell in tandem photovoltaic devices. However, theoptoelectronic quality of selenium thin-films has been identified as a keybottleneck for realizing high-efficiency selenium solar cells. In this study,we present a novel approach for crystallizing selenium thin-films usinglaser-annealing as an alternative to the conventionally used thermal annealingstrategy. By laser-annealing through a semitransparent substrate, a buriedlayer of high-quality selenium crystallites is formed and used as a growthtemplate for solid-phase epitaxy. The resulting selenium thin-films featurelarger and more preferentially oriented grains with a negligible surfaceroughness in comparison to thermally annealed selenium thin-films. We fabricatephotovoltaic devices using this strategy, and demonstrate a record idealityfactor of n=1.37, a record fill factor of FF=63.7%, and a power conversionefficiency of PCE=5.0%. The presented laser-annealing strategy is universallyapplicable and is a promising approach for crystallizing a wide range ofphotovoltaic materials where high temperatures are needed while maintaining alow substrate temperature.

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