Clustered Geometries Exploiting Quantum Coherence Effects for Efficient Energy Transfer in Light Harvesting

Abstract

Elucidating quantum coherence effects and geometrical factors for efficient energy transfer in photosynthesis has the potential to uncover non-classical design principles for advanced organic materials. We study energy transfer in a linear light-harvesting model to reveal that dimerized geometries with strong electronic coherences within donor and acceptor pairs exhibit significantly improved efficiency, which is in marked contrast to predictions of the classical Förster theory. We reveal that energy tuning due to coherent delocalization of photoexcitations is mainly responsible for the efficiency optimization. This coherence-assisted energy-tuning mechanism also explains the energetics and chlorophyll arrangements in the widely-studied Fenna-Matthews-Olson complex. We argue that a clustered network with rapid energy relaxation among donors and resonant energy transfer from donor to acceptor states provides a basic formula for constructing efficient light-harvesting systems, and the general principles revealed here can be generalized to larger systems and benefit future innovation of efficient molecular light-harvesting materials.

26 pages, 5 figures

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• Coherent and incoherent theories for photosynthetic energy transfer
• Exact and efficient quantum simulation of open quantum dynamics for various of Hamiltonians and spectral densities
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• Longitudinal relaxation of a nitrogen-vacancy center in a spin bath by generalized cluster-correlation expansion method
• Robust and fragile quantum effects in the transfer kinetics of delocalized excitons between B850 units of LH2 complexes
• Realizing Topological Transition in a Non-Hermitian Quantum Walk with Circuit QED
• Bringing quantum mechanics to life: from Schrödinger's cat to Schrödinger's microbe
• An efficient tool to calculate two-dimensional optical spectra for photoactive molecular complexes
• Artificial Light Harvesting by Dimerized Mobius Ring
• Quantum metrology with one auxiliary particle in a correlated bath and its quantum simulation
• Quantum simulation of clustered photosynthetic light harvesting in a superconducting quantum circuit
• Proposal for probing energy transfer pathway by single-molecule pump-dump experiment
• Simulation of non-radiative energy transfer in photosynthetic systems using a quantum computer
• Multi-Radical Lipkin-Meshkov-Glick Model for Avian Navigation
• Optical Non-Reciprocity in Coupled Resonators Inspired by Photosynthetic Energy Transfer