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Journal of the Optical Society of America B

Transfer efficiency in a pulsed light-harvesting trimer system

Ethan Wyke, Abuenameh Aiyejina, Roger Andrews, Andrew D. Greentree

Published May 29, 2024• 3 citations
Publisher

Abstract

In this paper, the theory of the transfer efficiency of a light-harvesting system consisting of a trimer ring coupled to an acceptor site is presented. When the ring has a prepared excitation or is excited using a laser pulse, the maximum transfer efficiency is approximately 0.5, while a near-perfect transfer efficiency is generated by a single photon. The near-perfect efficiency results from the creation of a dark state by the photon, which suppresses the effect of spontaneous decay from the donor.

DOI
10.1364/josab.523925

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In this paper, the theory of the transfer efficiency of a light-harvesting system consisting of a trimer ring coupled to an acceptor site is presented. When the ring has a prepared excitation or is excited using a laser pulse, the maximum transfer efficiency is approximately 0.5, while a near-perfect transfer efficiency is generated by a single photon. The near-perfect efficiency results from the creation of a dark state by the photon, which suppresses the effect of spontaneous decay from the donor.
We analytically derive transfer probabilities and efficiencies for an artificial light-harvesting photosynthetic system, which consists of a ring coupled to a central acceptor. For an incident photon pair, we find near-perfect single excitation transfer efficiency with negligible double excitation transfer in the weak-coupling regime. In the strong-coupling regime, single excitation transfer efficiency was greater than 9090%90, while the double excitation efficiency was approximately 5050%50. We have found that the three main factors which determine high transfer efficiencies are large acceptor probabilities, long acceptor decay times, and strong photon-ring coupling. A possible implementation of the theoretical framework to bio-inspired solar energy devices is also discussed.
The energy-transfer efficiency of the natural photosynthesis system seems to be perfectly optimized during the evolution for millions of years. However, how to enhance the efficiency in the artificial light-harvesting systems is still unclear. In this paper, we investigate the energy-transfer process in the photosystem I (PSI). When there is no effective coupling between the outer antenna (OA) and the reaction center (RC), the two light-harvesting networks are disconnected and thus the energy transfer is inefficient. In order to repair these disconnected networks, we introduce a bridge with three sites between them. We find that by modulating the level structure of the 3-site bridge to be resonant, the energy transfer via the dark state will be enhanced and even outperform the original PSI. Our discoveries may shed light on the designing mechanism of artificial light-harvesting systems.
We derive and simulate the wavefunctions and double-excitation probabilities for dimer and trimer three-level systems. Perfect state transfer occurs for pulse strengths that are odd multiples of π /2 when the parameter Jt equals odd multiples of π /2 and π /2 for the dimer and trimer, respectively. Near-perfect state transfer with a single photon occurred for photon coupling strength g =2 J when Jt=1.99,19.87 in the dimer and Jt=2.62,25.51 in the trimer. The nature of perfect state transfer is due to localization and transfer of double excitations for given pulse strengths and times.