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arXiv:2504.15172 · Physical Review A

Quantum excitation transfer in an artificial photosynthetic light-harvesting system

Stephon Alexander, Roger Andrews, Oliver Fox, Sarben Sarkar

Published Aug 4, 2025• 0 citations
arXivHTMLPDF

Abstract

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 $90%$, while the double excitation efficiency was approximately $50%$. 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.

DOI
10.1103/xyjw-lrf4

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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.
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.
The occurrence of coherence phenomenon as a result of the interference of the probability amplitude terms is among the principle features of quantum mechanics concepts. Current experiments display the presence of quantum techniques whose coherence is supplied over large interval times. Specifically, photosynthetic mechanisms in light-harvesting complexes furnish oscillatory behaviors owing to quantum coherence. In this manuscript, we study the coherent quantum energy transfer for a single-excitation and nonlocal correlation in a dimer system (donor+acceptor) displayed by two-level systems (TLSs), interacting with a cavity field with a time-dependent coupling effect considering the realistic situation of coupling between each TLS and the cavity field. We analyze and explore the specific conditions which are viable with real experimental realization for the ultimate transfer of quantum energy and nonlocal quantum correlation. We show that the enhancement of the probability for a single-excitation energy transfer greatly benefits from the energy detuning, photon-number transition, classicality of the field, and the time-dependent coupling effect. We also find that the entanglement between the donor and acceptor is very sensitive to the physical parameters and it can be generated during the coherent energy transfer.
Abstract Near-unity energy transfer efficiency has been widely observed in natural photosynthetic complexes. This phenomenon has attracted broad interest from different fields, such as physics, biology, chemistry, and material science, as it may offer valuable insights into efficient solar-energy harvesting. Recently, quantum coherent effects have been discovered in photosynthetic light harvesting, and their potential role on energy transfer has seen the heated debate. Here, we perform an experimental quantum simulation of photosynthetic energy transfer using nuclear magnetic resonance (NMR). We show that an N-chromophore photosynthetic complex, with arbitrary structure and bath spectral density, can be effectively simulated by a system with log2N qubits. The computational cost of simulating such a system with a theoretical tool, like the hierarchical equation of motion, which is exponential in N, can be potentially reduced to requiring a just polynomial number of qubits N using NMR quantum simulation. The benefits of performing such quantum simulation in NMR are even greater when the spectral density is complex, as in natural photosynthetic complexes. These findings may shed light on quantum coherence in energy transfer and help to provide design principles for efficient artificial light harvesting.
Photosystem I (PSI) is one of the most efficient natural photosynthetic complexes and serves as a structural prototype for understanding excitation energy transfer (EET) and designing artificial light-harvesting systems. Here, we construct a multilayer elliptical-conical quantum network inspired by PSI to investigate how antenna architecture affects EET. Excitation dynamics are simulated using the quantum jump approach combined with coherent modified Redfield theory (QJA-CMRT). The transfer efficiency exhibits a pronounced nonmonotonic dependence on pigment density, reaching a maximum of 0.86 at x=6 in the five-layer network. The optimal configuration contains 91 pigments, close to the number of core antenna pigments in natural PSI. Our combined density-of-states and kinetic analyses reveal that this nonmonotonic dependence originates from a trade-off: at low pigment densities, enhanced band overlap promotes energy transfer, whereas at high densities, excessive exciton delocalization compromises funnel directionality and reduces efficiency; the optimal configuration is consequently achieved at x=6. These findings provide insights into PSI antenna organization and offer guidelines for designing efficient artificial light-harvesting systems.
We investigate the role of non-Markovian effects in the efficiency of excitation transfer in a ring-hub arrangement of interacting two-level systems coupled to an environment. The structure is similar to light-harvesting antennae connected to a reaction centre as it is found in natural photosynthetic systems. To this order, we use stochastic Schrödinger equations within the so-called post-Markov approximation, which under certain constraints allows us to describe the system beyond the Markov and the weak-coupling approximations commonly used in the literature.
Networks of interacting molecular optical dipoles play an important role in photosynthetic light harvesting, and also hold significant promise for future artificial technologies. This manuscript gives a brief overview of questions addressed by (our) recent theoretical work with a focus on taking inspiration from biological structures and processes to come up with designs for utilising bio-inspired collective quantum optical effects. These could, for instance, enable quantum-enhanced light harvesting, the charging of Dicke quantum batteries through superabsorption of light, and achieving efficient long-range energy transport. Particular attention is given to the role of inter-emitter quantum coherence as an enabler of these effects.