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arXiv:2512.12660

Quantum Correlation and Synchronisation-Enhanced Energy Transfer in Driven-Dissipative Light-Harvesting Dimers

Wenhao Xu

physics.bio-phquant-phSubmitted Dec 14, 2025• Announced Dec 16, 2025• Revised Dec 28, 2025 (v2)
v1 · Dec 14, 2025v2 · Dec 28, 2025
arXivHTMLPDF

Abstract

Quantum synchronisation has recently been proposed as a mechanism for electronic excitation energy transfer in light-harvesting complexes, yet its robustness in driven-dissipative settings remains under active investigation. Here, we revisit this mechanism in cryptophyte photosynthetic antennae using an exciton--vibrational dimer model. By comparing the full open quantum dynamics with semi-classical rate equations for electronic density-matrix elements and vibrational observables, we demonstrate that quantum correlations between electronic and vibrational degrees of freedom, beyond the semi-classical factorised limit, underpin the emergence of quantum synchronisation. Furthermore, we introduce an environment-assisted transfer mechanism arising as a nonlinear, non-Condon correction to the dipole--dipole interaction. This mechanism enables long-lived quantum coherence and continuous, synchronisation-enhanced energy transfer in a driven-dissipative regime, thereby suggesting new avenues for investigating photosynthetic energy-transfer dynamics.

DOI
10.1016/j.mtquan.2026.100059

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Quantum synchronisation has recently been proposed as a mechanism for electronic excitation energy transfer in light-harvesting complexes, yet its robustness in driven-dissipative settings remains under active investigation. Here, we revisit this mechanism in cryptophyte photosynthetic antennae using an exciton--vibrational dimer model. By comparing the full open quantum dynamics with semi-classical rate equations for electronic density-matrix elements and vibrational observables, we demonstrate that quantum correlations between electronic and vibrational degrees of freedom, beyond the semi-classical factorised limit, underpin the emergence of quantum synchronisation. Furthermore, we introduce an environment-assisted transfer mechanism arising as a nonlinear, non-Condon correction to the dipole--dipole interaction. This mechanism enables long-lived quantum coherence and continuous, synchronisation-enhanced energy transfer in a driven-dissipative regime, thereby suggesting new avenues for investigating photosynthetic energy-transfer dynamics.
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The study of quantum phenomena in biology has received significant attention in the last decade. One of the problems of most interest is the understanding of quantum effects during the first steps of photosynthesis. Ultrafast two-dimensional electronic spectroscopy has revealed that pigment-protein complexes responsible for light- harvesting and charge separation in photosynthetic organisms can support quantum coherent dynamics in the excited state, for up to few hundreds of femtoseconds. The leading hypothesis on the mechanisms supporting this coherent behaviour is quan- tum interactions between electronic and some specific vibrational motions in the excited state. This hypothesis, however, awaits unambiguous confirmation. Among the most powerful techniques to investigate the quantum behaviour of an emitter is the study of quantum optical properties of the light it emits. This thesis de- velops theoretical studies showing that frequency-filtered and time-resolved photon counting statistics of the light emitted by a prototype photosynthetic unit can give important insight into the quantum coherent nature and the mechanisms underlying excited state dynamics in single photosynthetic complexes. By developing a pertur- bative and efficient approach to the computation of frequency- and time- resolved photon correlation functions, we show that such correlations have the potential to give unambiguous signatures of coherence contributions to the steady state emis- sion. For a light-harvesting unit emitting in free space, the signatures of excited state coherence manifest themselves as non-trivial antibunching. This feature can- not be probed by measuring unfiltered photon correlations. We then consider the situation in which a prototype energy transfer unit is embedded in an optical cavity such that its emission rate is enhanced. In this case we observed a rich behaviour of the frequency-filtered, second-order photon correlations that allows a clear distinc- tion of coherence contributions, and their variation, depending of the electronic and vibrational interactions in the system of interest.
Excitation-energy transfer underpins the conversion of light into usable energy in photosynthetic organisms and serves as a paradigm for evolutionary optimized transport in open quantum systems. Although this process is often described as incoherent thermally assisted hopping, such descriptions become inadequate when electronic coupling, vibronic interactions and environmental fluctuations occur on comparable energy scales. Determining how the environment controls transport therefore remains a fundamental challenge. Here, we use temperature-dependent 2DES to investigate energy transfer in the photosynthetic antenna protein allophycocyanin over the range 10 - 296 K. The dominant β→αβ\rightarrow αβ→α transfer step exhibits a pronounced non-monotonic temperature dependence: the transfer time decreases from 400 fs at 10 K to 200 fs near 30- 40 K before increasing again to 400 fs at 296 K. In contrast, the homogeneous optical dephasing time decreases monotonically across the same temperature range. To interpret these observations, we model APC as a vibronically coupled excitonic dimer interacting with a structured environment and solve the dynamics using hierarchical equations of motion. Conventional fixed-bath models, including Drude-Lorentz and explicit intermolecular-mode spectral densities, fail to reproduce the observed turnover. Quantitative agreement is obtained only when the low-frequency sector of the environmental spectral density is allowed to anharmonically evolve strongly with temperature, while the high-frequency bath remains essentially unchanged. More broadly, these findings demonstrate that transport efficiency is controlled not simply by the magnitude of environmental fluctuations, but by the distribution of environmental spectral weight across frequency space, providing new experimental constraints on theories of molecular transport in complex quantum environments.
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Ultrafast spectroscopy experiments show that photosynthetic systems can preserve quantum beats in the process of electronic energy transfer between pigments, even at room temperature. But what does this discovery imply for biology - and for quantum mechanics? This dissertation examines photosynthesis through the tools of quantum information science. We evaluate to what extent photosynthesis can be thought of as a type of quantum technology, and consider how we can apply experimental tools widely used for quantum technologies (state tomography and coherent control) to photosynthesis. Throughout, we use the Fenna-Matthews-Olson (FMO) complex of greens sulfur bacteria as a model photosynthetic pigment-protein complex.In Part I, we evaluate two mechanisms for the possible biological relevance of quantum coherent motion. First, we consider the extent to which dynamics in light-harvesting systems exhibit the quantum speedups characteristic of quantum algorithms and quantum walks. Second, we demonstrate a ratchet effect in electronic energy transfer enabled by partially coherent dynamics. To do so, we build a new model of energy transfer between weakly coupled light-harvesting complexes to understand how electronic coherence arises under natural conditions.In Part II, we present proposals for experimental probes of light harvesting dynamics with ultrafast spectroscopy. We show how the signal from pump-probe spectroscopy can be formally inverted to determine the excited state electronic density matrix. Finally, we examine the feasiblity of coherent control experiments on light-harvesting systems, and provide two realistic targets feasible with present-day technology.
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.