Single Molecule Spectroscopy of Monomeric LHCII: Experiment and Theory

We derive approximate equations of motion for excited state dynamics of a multilevel open quantum system weakly interacting with light to describe fluorescence-detected single molecule spectra. Based on the Frenkel exciton theory, we construct a model for the chlorophyll part of the LHCII complex of...

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Main Authors:	Malý, Pavel, Gruber, J. Michael, van Grondelle, Rienk, Mančal, Tomáš
Format:	Online
Language:	English
Published:	Nature Publishing Group 2016
Online Access:	https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4870570/

id	pubmed-4870570
recordtype	oai_dc
spelling	pubmed-48705702016-06-01 Single Molecule Spectroscopy of Monomeric LHCII: Experiment and Theory Malý, Pavel Gruber, J. Michael van Grondelle, Rienk Mančal, Tomáš Article We derive approximate equations of motion for excited state dynamics of a multilevel open quantum system weakly interacting with light to describe fluorescence-detected single molecule spectra. Based on the Frenkel exciton theory, we construct a model for the chlorophyll part of the LHCII complex of higher plants and its interaction with previously proposed excitation quencher in the form of the lutein molecule Lut 1. The resulting description is valid over a broad range of timescales relevant for single molecule spectroscopy, i.e. from ps to minutes. Validity of these equations is demonstrated by comparing simulations of ensemble and single-molecule spectra of monomeric LHCII with experiments. Using a conformational change of the LHCII protein as a switching mechanism, the intensity and spectral time traces of individual LHCII complexes are simulated, and the experimental statistical distributions are reproduced. Based on our model, it is shown that with reasonable assumptions about its interaction with chlorophylls, Lut 1 can act as an efficient fluorescence quencher in LHCII. Nature Publishing Group 2016-05-18 /pmc/articles/PMC4870570/ /pubmed/27189196 http://dx.doi.org/10.1038/srep26230 Text en Copyright © 2016, Macmillan Publishers Limited http://creativecommons.org/licenses/by/4.0/ This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
repository_type	Open Access Journal
institution_category	Foreign Institution
institution	US National Center for Biotechnology Information
building	NCBI PubMed
collection	Online Access
language	English
format	Online
author	Malý, Pavel Gruber, J. Michael van Grondelle, Rienk Mančal, Tomáš
spellingShingle	Malý, Pavel Gruber, J. Michael van Grondelle, Rienk Mančal, Tomáš Single Molecule Spectroscopy of Monomeric LHCII: Experiment and Theory
author_facet	Malý, Pavel Gruber, J. Michael van Grondelle, Rienk Mančal, Tomáš
author_sort	Malý, Pavel
title	Single Molecule Spectroscopy of Monomeric LHCII: Experiment and Theory
title_short	Single Molecule Spectroscopy of Monomeric LHCII: Experiment and Theory
title_full	Single Molecule Spectroscopy of Monomeric LHCII: Experiment and Theory
title_fullStr	Single Molecule Spectroscopy of Monomeric LHCII: Experiment and Theory
title_full_unstemmed	Single Molecule Spectroscopy of Monomeric LHCII: Experiment and Theory
title_sort	single molecule spectroscopy of monomeric lhcii: experiment and theory
description	We derive approximate equations of motion for excited state dynamics of a multilevel open quantum system weakly interacting with light to describe fluorescence-detected single molecule spectra. Based on the Frenkel exciton theory, we construct a model for the chlorophyll part of the LHCII complex of higher plants and its interaction with previously proposed excitation quencher in the form of the lutein molecule Lut 1. The resulting description is valid over a broad range of timescales relevant for single molecule spectroscopy, i.e. from ps to minutes. Validity of these equations is demonstrated by comparing simulations of ensemble and single-molecule spectra of monomeric LHCII with experiments. Using a conformational change of the LHCII protein as a switching mechanism, the intensity and spectral time traces of individual LHCII complexes are simulated, and the experimental statistical distributions are reproduced. Based on our model, it is shown that with reasonable assumptions about its interaction with chlorophylls, Lut 1 can act as an efficient fluorescence quencher in LHCII.
publisher	Nature Publishing Group
publishDate	2016
url	https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4870570/
_version_	1613580605965991936

Single Molecule Spectroscopy of Monomeric LHCII: Experiment and Theory

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