In the design of organic solar cells, there has been a need for materials with high power conversion efficiencies. Scharber's model is commonly used to predict efficiency; however, it exhibits poor performance with new non-fullerene acceptor (NFA) devices, since it was designed for fullerene-based devices. In this work, an empirical model is proposed that can be a more accurate alternative for NFA organic solar cells. Additionally, many screening studies use computationally expensive methods. A model based on using semiempirical simplified time-dependent density functional theory (sTD-DFT) as an alternative method can accelerate the calculations and yield a similar accuracy. The models presented in this paper, termed organic photovoltaic efficiency predictor (OPEP) models, have shown significantly lower errors than previous models, with OPEP/B3LYP yielding errors of 1.53% and OPEP/sTD-DFT of 1.55%. The proposed computational models can be used for the fast and accurate screening of new high-efficiency NFAs/donor pairs.

Materials optimization for organic solar cells (OSCs) is a highly active field, with many approaches using empirical experimental synthesis, computational brute-force approaches to screen candidates in a given subset of chemical space, or generative machine learning methods which often require significant training sets. While these methods may find high-performing materials, they can be inefficient and time-consuming. Genetic algorithms (GAs) are an alternative approach, allowing for the "virtual synthesis" of molecules and a prediction of their ``fitness' for some property, with new candidates suggested based on good characteristics of previously generated molecules. In this work, a GA is used to discover high-performing unfused non-fullerene acceptors (NFAs) based on an empirical prediction of power conversion efficiency (PCE) and provides design rules for future work. The electron withdrawing/donating strength, as well as the sequence and symmetry of those units are examined. The utilization of a GA over a brute force approach resulted in speedups up to $1.8 \times 10^{12}$. New types of units not frequently seen in OSCs are suggested, and in total 5,426 NFAs are discovered with the GA. Of these, 1,087 NFAs are predicted to have a PCE greater than 18\%, which is roughly the current record efficiency. While the symmetry of the sequence showed no correlation with PCE, analysis of the sequence arrangement revealed that higher performance can be achieved with a donor core and acceptor end groups. Future NFA designs should consider this strategy as an alternative to the current A-D-A$'$-D-A architecture.

Tandem organic solar cells can potentially drastically improve the power conversion efficiency over single-junction devices. However, there is limited research on device development and often ca. 1% improvement over single-junction devices. Because of the complex nature of organic material compatibility and properties, such as energy-level alignment and maximizing absorption spectra, and the vastness of chemical space, computational guidance is vital. The first part of this work uses a new data set of 1225 donor/non-fullerene acceptor (NFA) pairs containing 1001 unique pairs, one of the largest to date, to train an ensemble machine learning model to predict device efficiency (RMSE = 1.60 ± 0.14%). Next, a series of genetic algorithms (GAs) are used to discover high-performing NFAs and polymer donors and then combinations of them for potential high-efficiency tandem cells. Interesting design motifs show up in high-performing NFAs, such as diphenylamine substituents on the core and 3D terminal groups. The donor polymers from the GAs reveal that arranging the monomers as a smallblock copolymer may be beneficial instead of the typical alternating copolymer. The GAs for selecting tandem cell materials successfully find material combinations that, when in a device together, have strong absorption across the entire visible−near-IR spectrum. Computational guidance is critical for the selection of tandem OSC materials, with genetic algorithms proving a highly successful technique.

Materials optimization for organic solar cells (OSCs) is a highly active field, with many approaches using empirical experimental synthesis, computational brute-force approaches to screen candidates in a given subset of chemical space, or generative machine learning methods which often require significant training sets. While these methods may find high- performing materials, they can be inefficient and time-consuming. Genetic algorithms (GAs) are an alternative approach, allowing for the "virtual synthesis" of molecules and a prediction of their “fitness” for some property, with new candidates suggested based on good characteristics of previously generated molecules. In this work, a GA is used to discover high-performing unfused non-fullerene acceptors (NFAs) based on an empir- ical prediction of power conversion efficiency (PCE) and provides design rules for future work. The electron withdrawing/donating strength, as well as the sequence and symmetry of those units are examined. The utilization of a GA over a brute force approach resulted in speedups up to 1.8 × 1012. New types of units not frequently seen in OSCs are suggested, and in total 5,426 NFAs are discovered with the GA. Of these, 1,087 NFAs are predicted to have a PCE greater than 18%, which is roughly the current record efficiency. While the symmetry of the sequence showed no correlation with PCE, analysis of the sequence arrangement revealed that higher performance can be achieved with a donor core and ac- ceptor end groups. Future NFA designs should consider this strategy as an alternative to the current A-D-A′-D-A architecture.

Genetic algorithms (GAs) are a powerful tool to search large chemical spaces for inverse molecular design. However, GAs have multiple hyperparameters that have not been thoroughly investigated for chemical space searches. In this work, we examine the general effects of a number of hyperparameters, such as population size, elitism rate, selection method, mutation rate, and convergence criteria, on key GA performance metrics. We show that using a self-termination method with a minimum Spearman's rank correlation coefficient of 0.8 between generations maintained for 50 consecutive generations along with a population size of 32, 50% elitism rate, 3- way tournament selection, and a 40% mutation rate provides the best balance of finding the overall champion, maintaining good coverage of elite targets, and improving relative speedup for general use in molecular design GAs.