Electronic Structure and Charge Transport at Heterogeneous Functional Interfaces in Solar Energy Conversion Devices

Solar energy conversion devices are pivotal for the ongoing ecological transition toward a sustainable economic and social development. From re-emerging dye-sensitized solar cells for indoor light-recycling and building integrated photovoltaics [1] to the high-performance perovskite solar cells [2], the conversion of light into electricity involves charge transport across several constituent materials. The heterogeneous functional interfaces among these different materials are key for an efficient and effective conversion process. In this context, the complexity of multi-layered devices hinders a complete and conclusive understanding based on experimental outcomes. For this reason, computational modeling tools based on atomistic and first-principles approaches are at the forefront in the current revolution of materials design and optimization.<br/>Here we will discuss how DFT-based approaches are able to unveil the charge transfer mechanism in several interfaces between optically-active materials and charge-collector layers in different electrochemical environments: (i) at hybrid solid-liquid interface with promising Cu-based molecular redox-couples in dye sensitized photo-anodes [3] and (ii) at heterogenous interface between lead halide perovskite and molecular/inorganic hole transport materials [4,5] and passivation ligands [6].<br/>Our results provide new insights on the structure-property-functional relationships of different functional materials/interfaces and outline new design principles for further improvements of the corresponding devices.<br/> <br/>[1] AB Muñoz-García, I Benesperi , G. Boschloo, JJ Concepcion, JH Delcamp, EA Gibson, GJ Meyer, M Pavone, H Pettersson, A Hagfeldt, M Freitag<br/>2021 <u>Chem</u><u>ical Society Reviews</u> 50, 12450-12550<br/> <br/>[2] J Young Kim, J-W Lee, H Suk Jung, H Shin, N-G Park<br/>2020 <u>Chem</u><u>ical</u><u> Rev</u><u>iew</u> 120, 7867–7918<br/> <br/>[3] I Benesperi, H Michaels, T Edvinsson, M Pavone, MR Probert, P Waddel, AB Muñoz-García, M Freitag<br/>2022 <u>Chem</u> 8, 439-449<br/> <br/>[4] A Pecoraro, A De Maria, PD Veneri, M Pavone, AB Muñoz-García<br/>2020 <u>Physical Chemistry Chemical Physics</u> 22, 28401-28413<br/> <br/>[5] C Coppola, A Pecoraro, AB Muñoz-García, R Infantino, A Dessì, G Reginato R Basosi, A Sinicropi M Pavone<br/>2022 <u>Physical Chemistry Chemical Physics</u> https://doi.org/10.1039/D2CP01270G<br/> <br/>[6] R Grisorio, F Fasulo, AB Muñoz-García, M Pavone, D Conelli, E Fanizza, M Striccoli, I Allegretta, R Terzano, NMargiotta, P Vivo, GP Suranna<br/>2022 <u>Nano Letters</u> 22, 4437–4444