  Using a representative translational dimer model, high throughput
calculations are implemented for fast screening of a total of 74
diacenaphtho-extended heterocycle (DAH) derivatives as hole transport layer
(HTL) materials in perovskite solar cells (PVSCs). Different electronic
properties, including band structures, band gaps, and band edges compared to
methylammonium and formamidinium lead iodide perovskites, along with
reorganization energies, electronic couplings, and hole mobilities are
calculated in order to decipher the effects of different parameters, including
the polarity, steric and pi-conjugation, as well as the presence of explicit
hydrogen bond interactions on the computed carrier mobilities of the studied
materials. Full crystal structure predictions and hole mobility calculations of
the top candidates resulted in some mobilities exceeding 10 cm2/V.s, further
validating the employed translational dimer model as a robust approach for
inverse design and fast high throughput screening of new HTL organic
semiconductors with superior properties. The studied models and simulations
performed in this work are instructive in designing next-generation HTL
materials for higher-performance PVSCs.
