How to regulate energy levels and hole mobility of spiro-type hole transport materials in perovskite solar cells

Methoxyaniline-based organic small molecules with three-dimensional structure have been proven as the most promising hole conductor for state-of-the-art perovskite devices. A fundamental understanding of the electronic properties and hole transport behavior of spiro-CPDT analogues, which is dependent on the number and position of the -OCH₃ groups, is significant for their potential applications as hole transport materials of perovskite solar cells. Our results from density functional theory calculations indicate that meta-substitution is more beneficial to reduce the highest occupied molecular orbital (HOMO) levels of molecules compared with ortho- and para-substitution. Furthermore, the hole mobility can be improved by ortho-substitution or mixed ortho- and para-substitution. Most interestingly, it is found that the improvement in hole mobility is at the expense of raising the HOMO level of spiro-CPDT analogues. These results can be useful in the process of designing and synthesizing excellent hole transport materials with suitable HOMO levels and high hole mobility.