Elemental
selenium is an interesting candidate for the
top cell
in tandem solar cells due to its wide bandgap of E
G ≈ 1.95 eV as well as its monatomic simplicity.
To realize high-efficiency selenium solar cells, it is crucial to
optimize the crystallization process of the selenium thin-film photoabsorber.
However, the high vapor pressure of selenium restricts the processing
conditions to a compromise between the growth of large crystal grains
and the formation of pinholes. In this study, we introduce a closed-space
annealing (CSA) strategy designed to suppress the sublimation of selenium,
enabling thermal annealing processes at higher temperatures and for
longer periods of time. As a result, we consistently improve the carrier
collection and the overall photovoltaic device performance in our
selenium solar cells. By characterizing the carrier dynamics in our
devices, we conclude that the observed improvements result from a
reduction in the charge-transfer resistance rather than an increase
in the carrier diffusion length. The CSA strategy is a promising method
for controlling the surface morphology and roughness without reducing
crystal grain sizes, which paves the way for further advancements
in the efficiency and reproducibility of selenium thin-film solar
cells.