Probing the Effect of Acceptor Moiety Engineering in Carbazole‐Based Hole‐Transporting Materials for Efficient Perovskite Solar Cells

Abstract Computational studies on the relationship between the molecular structures and properties of hole‐transporting materials (HTMs) are an effective way to find promising HTMs for high‐performance perovskite solar cells (PSCs). Herein, a series of carbazole‐based five HTMs with diphenyl pyridine‐based side arms (namely CDPC , CDPP , CDPI , CDPT , and CDPM ) are designed. The results indicated that designed HTMs have deeper HOMO & LUMO levels, high absorption coefficient, low recombination rate, superior solubility, and comparable stability compared to the reference molecule which is based on carbazole diphenyl pyridine ( CDP ) for high‐efficiency perovskite solar cells (PSCs). The design molecules exhibit smaller exciton binding energies, which demonstrates that the electron‐hole pairs are easily dissociated into the free charge that facilitates the hole transport for PSCs. The results of low hole reorganization energy and the high total amount of charge transfer indicated that designed HTMs have effective hole transport ability. In the future, it is expected that this studies will demonstrate the potential of designed HTMs in the manufacture of effective PSCs in the solar industry.