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arXiv:0912.3560 · Physical Review E

Efficient and coherent excitation transfer across disordered molecular networks

Torsten Scholak, Fernando de Melo, Thomas Wellens, Florian Mintert, Andreas Buchleitner

Published Feb 22, 2011• 143 citations
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Abstract

We show that finite-size, disordered molecular networks can mediate highly efficient, coherent excitation transfer which is robust against ambient dephasing and associated with strong multisite entanglement. Such optimal, random molecular conformations may explain efficient energy transfer in the photosynthetic Fenna-Matthews-Olson complex.

DOI
10.1103/physreve.83.021912

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We show that finite-size, disordered molecular networks can mediate highly efficient, coherent excitation transfer which is robust against ambient dephasing and associated with strong multisite entanglement. Such optimal, random molecular conformations may explain efficient energy transfer in the photosynthetic Fenna-Matthews-Olson complex.
Abstract The Fenna-Matthews-Olson light-harvesting complexes have become a center of attention due to their high excitation energy transfer efficiency, which may surpass 98%. Experimental results reveal the presence of quantum entanglement in the protein structure, which seems to be associated to such a remarkably high efficiency. Notably, Redfield and Lindblad master equations have been already used to model the chromophore excitation in the protein complex as well as its interactions with the environment. The entanglement arising during the process has been quantified through several measures. This work provides a short review of methods used to model the above described system. It is also discussed the introduction of two nonconventional measures addresed to quantify the emergent entanglement.
Recent evidence of electronic coherence during energy transfer in photosynthetic antenna complexes has reinvigorated the discussion about whether coherence and/or entanglement have any practical functionality for these molecular systems. Here we investigate quantitative relationships between the quantum yield of a light-harvesting complex and the distribution of entanglement among its components. Our study focuses on the entanglement yield or average entanglement surviving a time scale comparable to the average excitation trapping time. We consider the Fenna–Matthews–Olson (FMO) protein of green sulfur bacteria as a prototype system and show that there is an inverse relationship between the quantum efficiency and the average entanglement between distant donor sites. Our results suggest that long-lasting electronic coherence among distant donors might help in the modulation of the light-harvesting function.
Partitioning the photonic environment into resonant and off-resonant modes provides a mechanism for dephasing suppression in photosynthetic energy transfer. Aligning the excitation spectrum with underdamped vibronic resonances in the Fenna-Matthews-Olson (FMO) complex prepares vibronically dressed states with reduced coupling to dissipative fluctuations, inducing a biexponential coherence decay: a rapid initial dephasing (τfast {\approx} 37fs) followed by persistent inter-band coherences extending beyond 1ps-a > 3x extension of the effective coherence window relative to broadband excitation (τc = 280fs). This improves forward transfer yields by 39% at 295K. PT-HOPS/SBD simulations establish that dual-band filtering at 750nm and 820nm targets vibronic resonances while bypassing dephasing-dominated noise. This enhancement is robust against static disorder (σ = 50 cm-1), with an ensemble-averaged increase of η = 0.39 {\pm} 0.04. These results identify selective vibronic excitation as a foundational design principle for coherence-assisted transport. This framework extends to symbiotic agrivoltaic systems, where organic photovoltaics function as active spectral filters to co-optimize excitonic transport alongside the photosynthetic requirements of underlying crops.
We investigate coherent and incoherent excitation transfer in a random network with dipole–dipole interactions as a model system describing energy transport, e.g., in photosynthetic light-harvesting complexes or gases of cold Rydberg atoms. For this purpose, we introduce and compare two different measures (the maximum output probability and the average transfer time) for the efficiency of transport from the input to the output site. We especially focus on optimal configurations which maximize the transfer efficiency and the impact of dephasing noise on the transport dynamics. For most configurations of the random network, the transfer efficiency increases when adding noise, giving rise to essentially classical transport. These noise-assisted configurations are, however, systematically less efficient than the optimal configurations. The latter reach their highest efficiency for purely coherent dynamics, i.e. in the absence of noise. 1.
Abstract We study the excitation transfer across a fully connected quantum network whose sites energies can be artificially designed. Starting from a simplified model of a broadly-studied physical system, we systematically optimize its local energies to achieve high excitation transfer for various environmental conditions, using an adaptive Gradient Descent technique and Automatic Differentiation. We show that almost perfect transfer can be achieved with and without local dephasing, provided that the dephasing rates are not too large. We investigate our solutions in terms of resilience against variations in either the network connection strengths, or size, as well as coherence losses. We highlight the different features of a dephasing-free and dephasing-driven transfer. Our work gives further insight into the interplay between coherence and dephasing effects in excitation-transfer phenomena across fully connected quantum networks. In turn, this will help designing optimal transfer in artificial open networks through the simple manipulation of local energies.
Abstract Quantum effects in photosynthetic energy transport in nature, especially for the typical Fenna-Matthews-Olson (FMO) complexes, are extensively studied in quantum biology. Such energy transport processes can be investigated as open quantum systems that blend the quantum coherence and environmental noise, and have been experimentally simulated on a few quantum devices. However, the existing experiments always lack a solid quantum simulation for the FMO energy transport due to their constraints to map a variety of issues in actual FMO complexes that have rich biological meanings. Here we successfully map the full coupling profile of the seven-site FMO structure by comprehensive characterisation and precise control of the evanescent coupling of the three-dimensional waveguide array. By applying a stochastic dynamical modulation on each waveguide, we introduce the base site energy and the dephasing term in coloured noise to faithfully simulate the power spectral density of the FMO complexes. We show our photonic model well interprets the phenomena including reorganisation energy, vibrational assistance, exciton transfer and energy localisation. We further experimentally demonstrate the existence of an optimal transport efficiency at certain dephasing strength, providing a window to closely investigate environment-assisted quantum transport.