From Molecules to Devices: A Multiscale Approach to Evaluating Organic Photovoltaics.

Due to their efficient molecular design, nonfullerene acceptors (NFAs) have significantly advanced organic photovoltaics (OPVs). However, the lack of models to screen and evaluate candidate NFAs based on the resulting device performance has impeded the rapid development of high-performance molecules. This work introduces a computational framework utilizing a kinetic Monte Carlo (kMC) model to derive device parameters from molecular properties computed through first principles. By analyzing the quantum chemical properties of diverse dimeric conformers, we estimate the relative probabilities of microscopic processes such as charge separation, recombination, and transport along with charge transfer state formation in the active layer of OPVs. These probabilities set up a random walk of charge carriers in a grid with disordered molecular sites, allowing us to track their average behavior and calculate key device parameters. Our model consistently predicts measured device parameters, including the short-circuit current and open-circuit voltage, for OPVs with diverse NFAs with high accuracy. Additionally, we applied the model to evaluate donor-acceptor combinations of known compounds and newly designed NFA molecules, identifying high-performing pairs. This model offers a computationally efficient approach for designing novel NFA molecules and optimizing the OPV performance.