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Quantumness in light harvesting is determined by vibrational dynamics

DOI:10.1063/1.5058136 期刊:The Journal of Chemical Physics 出版年份:2018 更新时间:2025-09-23 15:23:52
摘要: We demonstrate for the multi-level spin-boson (MLSB) Hamiltonian, typically used to describe biological light-harvesting, that the distinction between quantum and classical dynamics is determined entirely by the thermal environment. In particular, any MLSB model featuring classical interactions with a classical bath is exactly equivalent in its absorption and energy transfer dynamics to a classical model involving coupled harmonic oscillators. This result holds in the linear response regime for both pulsed and incoherent excitation. In the biological context, this finding highlights the centrality of vibrational dynamics in determining the 'quantumness' of photosynthetic light-harvesting, particularly in the creation of the photosynthetic energy funnel where excitation energy concentrates near the reaction center via a series of downhill energy transfer events. These findings support the idea that this energy funnel is exclusively quantum-mechanical in origin, although it need not rely on entanglement.
作者: Mike Reppert,Paul Brumer
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To demonstrate that the distinction between quantum and classical dynamics in light-harvesting is determined by the thermal environment, specifically vibrational dynamics, and to show that quantum effects are essential for the photosynthetic energy funnel.

The research concludes that quantum effects in light-harvesting arise from the quantized nature of vibrational dynamics, not from electronic coherence preservation. The photosynthetic energy funnel is identified as a quantum-mechanical phenomenon that does not require entanglement, emphasizing the role of quantum thermodynamics in energy localization.

The study is limited to theoretical models (MLSB and classical harmonic oscillators) and assumes weak excitation and partial adiabatic separation. It does not account for experimental validation or real-world complexities such as non-harmonic baths or multi-excitation dynamics. The findings may not fully capture all aspects of biological light-harvesting systems.

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