Publication date: 15th December 2025
The remarkable recent advances in photovoltaic energy conversion efficiency in molecular materials have resulted largely from the use of fused ring molecular acceptors that form strongly coupled domains in the solid state. These materials appear able to support efficient photocurrent generation with relatively small energetic offset between the ionization potential of donor and acceptor components, and the best performing molecular materials may even support charge pair generation in single material domains. In this work we investigate the behaviour of these materials by combining experimental measurements of charge generation in single-component and heterojunction devices with a computational model of the generation and evolution of delocalised excited states in such systems. We consider the influence of factors such as the nature of the charge separating heterojunction, molecular packing, energy and charge transport, electron-phonon coupling and loss pathways. We explore the impact of molecular parameters and find that low exciton reorganization energy and high and isotropic electronic coupling are important for efficient photogeneration. We go on to apply the same framework to polymer materials and tethered donor-acceptor structures. Finally, we will address the limits to energy conversion efficiency in such systems.
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