Quantum – coherent dynamics in photosynthetic charge separation revealed by wavelet analysis

Abstract Experimental/theoretical evidence for sustained vibration-assisted electronic (vibronic) coherence in the Photosystem II Reaction Center (PSII RC) indicates that photosynthetic solar-energy conversion might be optimized through the interplay of electronic and vibrational quantum dynamics. T...

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Autores principales:	Elisabet Romero, Javier Prior, Alex W. Chin, Sarah E. Morgan, Vladimir I. Novoderezhkin, Martin B. Plenio, Rienk van Grondelle
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2017
Materias:	Medicine R Science Q
Acceso en línea:	https://doaj.org/article/fe1ad5405324413cafc1782d9315fe57
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spelling	oai:doaj.org-article:fe1ad5405324413cafc1782d9315fe572021-12-02T16:07:59ZQuantum – coherent dynamics in photosynthetic charge separation revealed by wavelet analysis10.1038/s41598-017-02906-72045-2322https://doaj.org/article/fe1ad5405324413cafc1782d9315fe572017-06-01T00:00:00Zhttps://doi.org/10.1038/s41598-017-02906-7https://doaj.org/toc/2045-2322Abstract Experimental/theoretical evidence for sustained vibration-assisted electronic (vibronic) coherence in the Photosystem II Reaction Center (PSII RC) indicates that photosynthetic solar-energy conversion might be optimized through the interplay of electronic and vibrational quantum dynamics. This evidence has been obtained by investigating the primary charge separation process in the PSII RC by two-dimensional electronic spectroscopy (2DES) and Redfield modeling of the experimental data. However, while conventional Fourier transform analysis of the 2DES data allows oscillatory signatures of vibronic coherence to be identified in the frequency domain in the form of static 2D frequency maps, the real-time evolution of the coherences is lost. Here we apply for the first time wavelet analysis to the PSII RC 2DES data to obtain time-resolved 2D frequency maps. These maps allow us to demonstrate that (i) coherence between the excitons initiating the two different charge separation pathways is active for more than 500 fs, and (ii) coherence between exciton and charge-transfer states, the reactant and product of the charge separation reaction, respectively; is active for at least 1 ps. These findings imply that the PSII RC employs coherence (i) to sample competing electron transfer pathways, and ii) to perform directed, ultrafast and efficient electron transfer.Elisabet RomeroJavier PriorAlex W. ChinSarah E. MorganVladimir I. NovoderezhkinMartin B. PlenioRienk van GrondelleNature PortfolioarticleMedicineRScienceQENScientific Reports, Vol 7, Iss 1, Pp 1-8 (2017)
institution	DOAJ
collection	DOAJ
language	EN
topic	Medicine R Science Q
spellingShingle	Medicine R Science Q Elisabet Romero Javier Prior Alex W. Chin Sarah E. Morgan Vladimir I. Novoderezhkin Martin B. Plenio Rienk van Grondelle Quantum – coherent dynamics in photosynthetic charge separation revealed by wavelet analysis
description	Abstract Experimental/theoretical evidence for sustained vibration-assisted electronic (vibronic) coherence in the Photosystem II Reaction Center (PSII RC) indicates that photosynthetic solar-energy conversion might be optimized through the interplay of electronic and vibrational quantum dynamics. This evidence has been obtained by investigating the primary charge separation process in the PSII RC by two-dimensional electronic spectroscopy (2DES) and Redfield modeling of the experimental data. However, while conventional Fourier transform analysis of the 2DES data allows oscillatory signatures of vibronic coherence to be identified in the frequency domain in the form of static 2D frequency maps, the real-time evolution of the coherences is lost. Here we apply for the first time wavelet analysis to the PSII RC 2DES data to obtain time-resolved 2D frequency maps. These maps allow us to demonstrate that (i) coherence between the excitons initiating the two different charge separation pathways is active for more than 500 fs, and (ii) coherence between exciton and charge-transfer states, the reactant and product of the charge separation reaction, respectively; is active for at least 1 ps. These findings imply that the PSII RC employs coherence (i) to sample competing electron transfer pathways, and ii) to perform directed, ultrafast and efficient electron transfer.
format	article
author	Elisabet Romero Javier Prior Alex W. Chin Sarah E. Morgan Vladimir I. Novoderezhkin Martin B. Plenio Rienk van Grondelle
author_facet	Elisabet Romero Javier Prior Alex W. Chin Sarah E. Morgan Vladimir I. Novoderezhkin Martin B. Plenio Rienk van Grondelle
author_sort	Elisabet Romero
title	Quantum – coherent dynamics in photosynthetic charge separation revealed by wavelet analysis
title_short	Quantum – coherent dynamics in photosynthetic charge separation revealed by wavelet analysis
title_full	Quantum – coherent dynamics in photosynthetic charge separation revealed by wavelet analysis
title_fullStr	Quantum – coherent dynamics in photosynthetic charge separation revealed by wavelet analysis
title_full_unstemmed	Quantum – coherent dynamics in photosynthetic charge separation revealed by wavelet analysis
title_sort	quantum – coherent dynamics in photosynthetic charge separation revealed by wavelet analysis
publisher	Nature Portfolio
publishDate	2017
url	https://doaj.org/article/fe1ad5405324413cafc1782d9315fe57
work_keys_str_mv	AT elisabetromero quantumcoherentdynamicsinphotosyntheticchargeseparationrevealedbywaveletanalysis AT javierprior quantumcoherentdynamicsinphotosyntheticchargeseparationrevealedbywaveletanalysis AT alexwchin quantumcoherentdynamicsinphotosyntheticchargeseparationrevealedbywaveletanalysis AT sarahemorgan quantumcoherentdynamicsinphotosyntheticchargeseparationrevealedbywaveletanalysis AT vladimirinovoderezhkin quantumcoherentdynamicsinphotosyntheticchargeseparationrevealedbywaveletanalysis AT martinbplenio quantumcoherentdynamicsinphotosyntheticchargeseparationrevealedbywaveletanalysis AT rienkvangrondelle quantumcoherentdynamicsinphotosyntheticchargeseparationrevealedbywaveletanalysis
_version_	1718384694546923520

Quantum – coherent dynamics in photosynthetic charge separation revealed by wavelet analysis

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