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Static Disorder has Dynamic Impact on Energy Transport in Biomimetic Light-Harvesting Complexes

[Image: see text] Despite extensive studies, many questions remain about what structural and energetic factors give rise to the remarkable energy transport efficiency of photosynthetic light-harvesting protein complexes, owing largely to the inability to synthetically control such factors in these n...

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Autores principales: Hamerlynck, Leo M., Bischoff, Amanda J., Rogers, Julia R., Roberts, Trevor D., Dai, Jing, Geissler, Phillip L., Francis, Matthew B., Ginsberg, Naomi S.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2022
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9574921/
https://www.ncbi.nlm.nih.gov/pubmed/36191182
http://dx.doi.org/10.1021/acs.jpcb.2c06614
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author Hamerlynck, Leo M.
Bischoff, Amanda J.
Rogers, Julia R.
Roberts, Trevor D.
Dai, Jing
Geissler, Phillip L.
Francis, Matthew B.
Ginsberg, Naomi S.
author_facet Hamerlynck, Leo M.
Bischoff, Amanda J.
Rogers, Julia R.
Roberts, Trevor D.
Dai, Jing
Geissler, Phillip L.
Francis, Matthew B.
Ginsberg, Naomi S.
author_sort Hamerlynck, Leo M.
collection PubMed
description [Image: see text] Despite extensive studies, many questions remain about what structural and energetic factors give rise to the remarkable energy transport efficiency of photosynthetic light-harvesting protein complexes, owing largely to the inability to synthetically control such factors in these natural systems. Herein, we demonstrate energy transfer within a biomimetic light-harvesting complex consisting of identical chromophores attached in a circular array to a protein scaffold derived from the tobacco mosaic virus coat protein. We confirm the capability of energy transport by observing ultrafast depolarization in transient absorption anisotropy measurements and a redshift in time-resolved emission spectra in these complexes. Modeling the system with kinetic Monte Carlo simulations recapitulates the observed anisotropy decays, suggesting an inter-site hopping rate as high as 1.6 ps(–1). With these simulations, we identify static disorder in orientation, site energy, and degree of coupling as key remaining factors to control to achieve long-range energy transfer in these systems. We thereby establish this system as a highly promising, bottom-up model for studying long-range energy transfer in light-harvesting protein complexes.
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spelling pubmed-95749212022-10-18 Static Disorder has Dynamic Impact on Energy Transport in Biomimetic Light-Harvesting Complexes Hamerlynck, Leo M. Bischoff, Amanda J. Rogers, Julia R. Roberts, Trevor D. Dai, Jing Geissler, Phillip L. Francis, Matthew B. Ginsberg, Naomi S. J Phys Chem B [Image: see text] Despite extensive studies, many questions remain about what structural and energetic factors give rise to the remarkable energy transport efficiency of photosynthetic light-harvesting protein complexes, owing largely to the inability to synthetically control such factors in these natural systems. Herein, we demonstrate energy transfer within a biomimetic light-harvesting complex consisting of identical chromophores attached in a circular array to a protein scaffold derived from the tobacco mosaic virus coat protein. We confirm the capability of energy transport by observing ultrafast depolarization in transient absorption anisotropy measurements and a redshift in time-resolved emission spectra in these complexes. Modeling the system with kinetic Monte Carlo simulations recapitulates the observed anisotropy decays, suggesting an inter-site hopping rate as high as 1.6 ps(–1). With these simulations, we identify static disorder in orientation, site energy, and degree of coupling as key remaining factors to control to achieve long-range energy transfer in these systems. We thereby establish this system as a highly promising, bottom-up model for studying long-range energy transfer in light-harvesting protein complexes. American Chemical Society 2022-10-03 2022-10-13 /pmc/articles/PMC9574921/ /pubmed/36191182 http://dx.doi.org/10.1021/acs.jpcb.2c06614 Text en © 2022 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Hamerlynck, Leo M.
Bischoff, Amanda J.
Rogers, Julia R.
Roberts, Trevor D.
Dai, Jing
Geissler, Phillip L.
Francis, Matthew B.
Ginsberg, Naomi S.
Static Disorder has Dynamic Impact on Energy Transport in Biomimetic Light-Harvesting Complexes
title Static Disorder has Dynamic Impact on Energy Transport in Biomimetic Light-Harvesting Complexes
title_full Static Disorder has Dynamic Impact on Energy Transport in Biomimetic Light-Harvesting Complexes
title_fullStr Static Disorder has Dynamic Impact on Energy Transport in Biomimetic Light-Harvesting Complexes
title_full_unstemmed Static Disorder has Dynamic Impact on Energy Transport in Biomimetic Light-Harvesting Complexes
title_short Static Disorder has Dynamic Impact on Energy Transport in Biomimetic Light-Harvesting Complexes
title_sort static disorder has dynamic impact on energy transport in biomimetic light-harvesting complexes
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9574921/
https://www.ncbi.nlm.nih.gov/pubmed/36191182
http://dx.doi.org/10.1021/acs.jpcb.2c06614
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