Steady-State Analysis of Light-harvesting Energy Transfer Driven by Incoherent Light: From Dimers to Networks

• URL: http://arxiv.org/abs/2007.10825v1
• Date: Sat, 18 Jul 2020 01:14:04 GMT
• Title: Steady-State Analysis of Light-harvesting Energy Transfer Driven by Incoherent Light: From Dimers to Networks
• Authors: Pei-Yun Yang and Jianshu Cao
• Abstract summary: We study how quantum coherence facilitates energy transfer under incoherent light. For light-harvesting systems under incoherent light, non-equilibrium energy transfer flux (i.e. steady-state coherence) is driven by the breakdown of detailed balance. It should be noted that the steady-state coherence or, equivalently, efficiency is the combined result of light-induced transient coherence, inhomogeneous depletion, and system-bath correlation.
• Score: 0.0
• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: The question of how quantum coherence facilitates energy transfer has been intensively debated in the scientific community. Since natural and artificial light-harvesting units operate under the stationary condition, we address this question via a non-equilibrium steady-state analysis of a molecular dimer irradiated by incoherent sunlight and then generalize the key predictions to arbitrarily-complex exciton networks. The central result of the steady-state analysis is the coherence-flux-efficiency relation:$\eta=c\sum_{i\neq j}F_{ij}\kappa_j=2c\sum_{i\neq j}J_{ij}{\rm Im}[{\rho}_{ij}]\kappa_j$ with $c$ the normalization constant. In this relation, the first equality indicates that energy transfer efficiency $\eta$ is uniquely determined by the trapping flux, which is the product of flux $F$ and branching ratio $\kappa$ for trapping at the reaction centers, and the second equality indicates that the energy transfer flux $F$ is equivalent to quantum coherence measured by the imaginary part of the off-diagonal density matrix, i.e., $F_{ij}=2J_{ij}{\rm Im}[{\rho}_{ij}]$. Consequently, maximal steady-state coherence gives rise to optimal efficiency. The coherence-flux-efficiency relation holds rigorously and generally for any exciton networks of arbitrary connectivity under the stationary condition and is not limited to incoherent radiation or incoherent pumping. For light-harvesting systems under incoherent light, non-equilibrium energy transfer flux (i.e. steady-state coherence) is driven by the breakdown of detailed balance and by the quantum interference of light-excitations and leads to the optimization of energy transfer efficiency. It should be noted that the steady-state coherence or, equivalently, efficiency is the combined result of light-induced transient coherence, inhomogeneous depletion, and system-bath correlation, and is thus not necessarily correlated with quantum beatings.

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