Spectroscopic elucidation of uncoupled transition energies in the major photosynthetic light-harvesting complex, LHCII.

Proceedings of the National Academy of Sciences of the United States of America
Gabriela S Schlau-CohenGraham R Fleming

Abstract

Electrostatic couplings between chromophores in photosynthetic pigment-protein complexes, and interactions of pigments with the surrounding protein environment, produce a complicated energy landscape of delocalized excited states. The resultant electronic structure absorbs light and gives rise to energy transfer steps that direct the excitation toward a site of charge separation with near unity quantum efficiency. Knowledge of the transition energies of the uncoupled chromophores is required to describe how the wave functions of the individual pigments combine to form this manifold of delocalized excited states that effectively harvests light energy. In an investigation of the major light-harvesting complex of photosystem II (LHCII), we develop a method based on polarized 2D electronic spectroscopy to experimentally access the energies of the S(0)-S(1) transitions in the chromophore site basis. Rotating the linear polarization of the incident laser pulses reveals previously hidden off-diagonal features. We exploit the polarization dependence of energy transfer peaks to find the angles between the excited state transition dipole moments. We show that these angles provide a spectroscopic method to directly inform on the relations...Continue Reading

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Citations

Nov 13, 2012·The Journal of Physical Chemistry. a·Jennifer E Laaser, Martin T Zanni
Apr 24, 2012·Nature Chemistry·Gabriela S Schlau-CohenGraham R Fleming
Feb 16, 2011·Proceedings of the National Academy of Sciences of the United States of America·Naomi S GinsbergGraham R Fleming
Sep 24, 2011·Proceedings of the National Academy of Sciences of the United States of America·Geoffrey A LottAndrew H Marcus
Nov 13, 2008·Annual Review of Physical Chemistry·Yuan-Chung Cheng, Graham R Fleming
Mar 8, 2013·The Review of Scientific Instruments·P DeyD Karaiskaj
Dec 5, 2012·The Journal of Chemical Physics·Jan RodenAlexander Eisfeld
Feb 20, 2016·The Journal of Physical Chemistry Letters·Nicholas H C Lewis, Graham R Fleming
Jun 9, 2015·Interface Focus·G S Schlau-Cohen
Apr 20, 2016·Annual Review of Physical Chemistry·Mi Kyung LeeDavid F Coker
Jul 30, 2016·The Journal of Physical Chemistry Letters·Mi Kyung Lee, David F Coker
Jan 11, 2017·Chemical Reviews·Toru KondoGabriela S Schlau-Cohen
Jun 16, 2015·Physical Chemistry Chemical Physics : PCCP·Pengfei Huo, Thomas F Miller
May 9, 2014·Physical Chemistry Chemical Physics : PCCP·Kym L WellsHowe-Siang Tan
Apr 16, 2015·Physical Chemistry Chemical Physics : PCCP·Sandro JurinovichBenedetta Mennucci
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Feb 8, 2018·Royal Society Open Science·Thomas A A Oliver
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Apr 5, 2012·Faraday Discussions·Graham R FlemingJulia Zaks
Apr 22, 2016·Angewandte Chemie·Dominika BednarczykDror Noy
Mar 21, 2020·Nature Communications·Eric A ArsenaultGraham R Fleming
Aug 16, 2017·Physical Chemistry Chemical Physics : PCCP·Charusheela RamananRienk van Grondelle
Aug 6, 2020·The Journal of Chemical Physics·Pallavi Bhattacharyya, Graham R Fleming
Jul 15, 2020·Physical Chemistry Chemical Physics : PCCP·Vladislav SlámaBenedetta Mennucci
Nov 28, 2020·Nature Communications·Eric A ArsenaultGraham R Fleming
Jul 10, 2021·The Journal of Chemical Physics·James D GaynorMunira Khalil
Sep 6, 2012·The Journal of Physical Chemistry Letters·Gabriela S Schlau-CohenGraham R Fleming
Apr 2, 2011·The Journal of Physical Chemistry. B·Tjaart P J KrügerRienk van Grondelle

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