Publication date: 11th March 2026
The energy conversion efficiency of photovoltaic devices based on molecular materials has improved remarkably to exceed 20% for many systems. These recent advances have resulted largely from the use of fused-ring molecular acceptors that absorb light strongly and form well 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 some systems appear to be capable of charge pair photogeneration without a heterojunction. To better understand such materials we investigate charge generation in single-component and heterojunction devices systematically for a range of materials, and analyse their behaviour using 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 [1]. We find that although some parameters favour charge separation in neat molecular domains, the ability of currently known materials to generate photocurrent efficiently without a heterojunction is limited. We go on to apply a similar framework to polymer materials and tethered donor-acceptor structures. The combined results allow us to consider the limits to energy conversion efficiency in such systems.
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