High-Throughput Screening, Crystal Structure Prediction, and Carrier Mobility Calculations of Organic Molecular Semiconductors as Hole Transport Layer Materials in Perovskite Solar Cells

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 π-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.