Electron-vibrational coupling decreases trapping by low-energy states in photosynthesis

Research output: Contribution to JournalArticleAcademicpeer-review

Abstract

In photosynthetic light harvesting, states with energy well below that needed for charge separation can be found in abundance. They do not hinder the quantum efficiency of the primary processes; on the contrary, they can be highly functional, extending the absorption towards the red. Although many properties of these states are well described based on spectroscopic and theoretical studies, the physical mechanisms underlying their working are not known. Here we propose a mechanism which utilizes high-frequency vibrations of the photosynthetic pigments and the combined spatio-energetic aspect of the excitation dynamics. We present numerical calculations of the excitation dynamics in explicit electron-vibrational basis, with parameters based on photosynthetic complexes such as the Lhca4 complex of higher plants. The electron-vibrational states have two roles. For the trapped, low-energy excitation they provide a thermally populated ladder out of the trap. And for the high-energy excitation they provide local-bath states, effectively forming a bridge over the trap.

Original languageEnglish
Pages (from-to)69-76
Number of pages8
JournalChemical Physics
Volume522
DOIs
Publication statusPublished - 1 Jun 2019

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photosynthesis
Photosynthesis
Excitation energy
Electron energy levels
trapping
Photosynthetic Reaction Center Complex Proteins
Electrons
Ladders
Quantum efficiency
Pigments
excitation
electrons
traps
energy
polarization (charge separation)
pigments
ladders
vibrational states
quantum efficiency
baths

Cite this

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title = "Electron-vibrational coupling decreases trapping by low-energy states in photosynthesis",
abstract = "In photosynthetic light harvesting, states with energy well below that needed for charge separation can be found in abundance. They do not hinder the quantum efficiency of the primary processes; on the contrary, they can be highly functional, extending the absorption towards the red. Although many properties of these states are well described based on spectroscopic and theoretical studies, the physical mechanisms underlying their working are not known. Here we propose a mechanism which utilizes high-frequency vibrations of the photosynthetic pigments and the combined spatio-energetic aspect of the excitation dynamics. We present numerical calculations of the excitation dynamics in explicit electron-vibrational basis, with parameters based on photosynthetic complexes such as the Lhca4 complex of higher plants. The electron-vibrational states have two roles. For the trapped, low-energy excitation they provide a thermally populated ladder out of the trap. And for the high-energy excitation they provide local-bath states, effectively forming a bridge over the trap.",
author = "Pavel Mal{\'y} and Novoderezhkin, {Vladimir I.} and {van Grondelle}, Rienk and Tom{\'a}š Mančal",
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Electron-vibrational coupling decreases trapping by low-energy states in photosynthesis. / Malý, Pavel; Novoderezhkin, Vladimir I.; van Grondelle, Rienk; Mančal, Tomáš.

In: Chemical Physics, Vol. 522, 01.06.2019, p. 69-76.

Research output: Contribution to JournalArticleAcademicpeer-review

TY - JOUR

T1 - Electron-vibrational coupling decreases trapping by low-energy states in photosynthesis

AU - Malý, Pavel

AU - Novoderezhkin, Vladimir I.

AU - van Grondelle, Rienk

AU - Mančal, Tomáš

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AB - In photosynthetic light harvesting, states with energy well below that needed for charge separation can be found in abundance. They do not hinder the quantum efficiency of the primary processes; on the contrary, they can be highly functional, extending the absorption towards the red. Although many properties of these states are well described based on spectroscopic and theoretical studies, the physical mechanisms underlying their working are not known. Here we propose a mechanism which utilizes high-frequency vibrations of the photosynthetic pigments and the combined spatio-energetic aspect of the excitation dynamics. We present numerical calculations of the excitation dynamics in explicit electron-vibrational basis, with parameters based on photosynthetic complexes such as the Lhca4 complex of higher plants. The electron-vibrational states have two roles. For the trapped, low-energy excitation they provide a thermally populated ladder out of the trap. And for the high-energy excitation they provide local-bath states, effectively forming a bridge over the trap.

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