Abstract
Photocells based on a simple optical transition suffer a fundamental efficiency threshold imposed by the principle of detailed balance, reflecting the fact that good absorbers must necessarily also be fast emitters. This limitation can be overcome by `parking' the energy of an absorbed photon in a `dark state' which neither absorbs nor emits light. Here we argue that suitable dark-states occur naturally as a consequence of the dipole-dipole interaction between two proximal optical dipoles for a wide range of realistic molecular dimers. We develop an intuitive model of a photocell comprising two light-absorbing molecules coupled to an idealised reaction centre, showing asymmetric dimers are capable of providing a significant enhancement of light-to-current conversion under ambient conditions. We conclude by presenting a host of candidate molecules meeting the requirements for realising such a system.
Original language | English |
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Article number | 203603 |
Journal | Physical Review Letters |
Volume | 117 |
Issue number | 20 |
DOIs | |
Publication status | Published - 10 Nov 2016 |
Keywords
- quant-ph
- physics.chem-ph
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Erik Gauger
- School of Engineering & Physical Sciences - Professor
- School of Engineering & Physical Sciences, Institute of Photonics and Quantum Sciences - Professor
Person: Academic (Research & Teaching)