Tetrathiafulvalene Derivatives as Hole-Transporting Materials in Perovskite Solar Cell

Over a couple of decades perovskite solar cells have become a highly promising photovoltaic technology. Choosing a dopant-free Hole-Transporting Material (HTM) that offers protection to a perovskite layer from oxidation is one of the viable strategies while addressing the stability of perovskite solar cell. In this line of interest, tetrathiafulvale (TTF) derivatives have shown promise in the past. However, studies that focus on small-molecule TTF derivatives as potential HTM options are scarce. The present study is an attempt to explore the applicability of a few TTF derivatives as HTM in a perovskite solar cell. Here four TTF derivatives, namely, TTF-1 (experimentally reported in a previous study), TTF-2, DBTTF1, and TMTSF1, were studied through electronic structure calculations. The properties concerning HTM, such as impact of adsorption on molecular structure, absorption spectra, distribution of frontier molecular orbitals, interaction energy between TTF derivative and MAPbI₃ surface, and charge transfer at an interface, were analyzed. Results show that TTF-2 has the expected energy-level alignment, transparency in the visible range of solar spectrum, and good charge-injection ability at the interface with a perovskite layer. Hence, TTF-2 could be a potential hole-transporting material for a perovskite solar cell, and it can perform better than TTF-1.