In‐Silico Device Performance Prediction of Cosensitizer Dye Pairs for Dye‐Sensitized Solar Cells

• Published in: Advanced energy materials Vol. 13; no. 6
• Main Authors: Devereux, Leon R., Vázquez‐Mayagoitia, Álvaro, Sternberg, Michael G., Cole, Jacqueline M.
• Format: Journal Article
• Language: English
• Published: 01.02.2023
• Subjects: cosensitization; density functional theory; dye‐sensitized solar cells; materials discovery; structure–property relationships
• ISSN: 1614-6832; 1614-6840
• DOI: 10.1002/aenm.202203536

Endeavors in the field of dye‐sensitized solar cells (DSCs) have shown great promise when adopting a data‐driven approach to materials discovery, such as successful molecular‐scale predictions of light‐harvesting chromophores. However, predictions of DSC dyes would become much more sophisticated if a molecular‐to‐macroscopic DSC device prediction methodology existed. Thereby, a fully computational pipeline is presented that predicts device‐performance parameters of DSCs which contain varying dye combinations. Optimal pairing of complementary dyes is identified via a data‐driven workflow that affords cosensitized DSCs with maximum power‐conversion efficiencies. Six high‐performing DSC dyes are paired with partner dyes that are screened from a database of 8488 compounds using sequential heuristic filters. Existing models that predict short‐circuit‐current density (JSC) and open‐circuit voltage (VOC) parameters are adapted to predict singly sensitized and cosensitized DSC performance. The predictions for Jsc values of singly sensitized devices match experimental literature values with comparable accuracy to more computationally costly methods. Five out of six dye pairings are predicted to have greater JSC values when cosensitized compared to their corresponding singly sensitized devices, including two pairs that show strong Jsc boosts of +13% and +12% when cosensitized. Thus, the prospect of an entirely in‐silico prediction pipeline for DSC performance that can be used to realize the fully automated design of optimized cosensitized DSCs is demonstrated. Concepts from data‐driven materials discovery are applied to optimization of cosensitization within dye‐sensitized solar cells (DSCs). High‐performing dyes are systematically paired up to complementary dyes from a database to achieve panchromatic absorption. Density functional theory and theoretical models are used to predict improvements to device performance parameters upon cosensitization of dye pairs. A full in‐silico design‐to‐device pipeline for DSCs is thus demonstrated.