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Autori principali: Liu, Jingyu, Du, Tao-Yuan
Natura: Preprint
Pubblicazione: 2026
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Accesso online:https://arxiv.org/abs/2603.29132
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author Liu, Jingyu
Du, Tao-Yuan
author_facet Liu, Jingyu
Du, Tao-Yuan
contents Photosynthetic antenna complexes achieve high quantum efficiency through exciton transport in coupled pigment networks. Conventional Frenkel-exciton models treat each chromophore as a structureless site and neglect internal electronic degrees of freedom that can influence coherence and delocalization. Here we develop an extended excitonic network model that preserves the pigment-pigment coupling topology while introducing tunable intrachromophoric electronic mixing within the single-excitation manifold. Using a Lindblad open-quantum-system framework, we quantify coherence, delocalization, and trapping efficiency across parameter space. We show that intrachromophoric mixing plays a time-dependent role: enhanced mixing on the antenna side promotes short-time coherent delocalization and improves excitation injection, whereas excessive mixing near the trapping site induces persistent delocalization and suppresses transfer efficiency. Simulated two-dimensional electronic spectra reveal enhanced cross peaks and systematic blue shifts, providing spectroscopic signatures of coherence-modulated transport. These results establish a microscopic connection between internal electronic structure and quantum transport performance in excitonic networks.
format Preprint
id arxiv_https___arxiv_org_abs_2603_29132
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Time-resolved role of coherence and delocalization in photosynthetic energy transfer from an extended exciton model
Liu, Jingyu
Du, Tao-Yuan
Optics
Quantum Physics
Photosynthetic antenna complexes achieve high quantum efficiency through exciton transport in coupled pigment networks. Conventional Frenkel-exciton models treat each chromophore as a structureless site and neglect internal electronic degrees of freedom that can influence coherence and delocalization. Here we develop an extended excitonic network model that preserves the pigment-pigment coupling topology while introducing tunable intrachromophoric electronic mixing within the single-excitation manifold. Using a Lindblad open-quantum-system framework, we quantify coherence, delocalization, and trapping efficiency across parameter space. We show that intrachromophoric mixing plays a time-dependent role: enhanced mixing on the antenna side promotes short-time coherent delocalization and improves excitation injection, whereas excessive mixing near the trapping site induces persistent delocalization and suppresses transfer efficiency. Simulated two-dimensional electronic spectra reveal enhanced cross peaks and systematic blue shifts, providing spectroscopic signatures of coherence-modulated transport. These results establish a microscopic connection between internal electronic structure and quantum transport performance in excitonic networks.
title Time-resolved role of coherence and delocalization in photosynthetic energy transfer from an extended exciton model
topic Optics
Quantum Physics
url https://arxiv.org/abs/2603.29132