A Quantum Chemical Interpretation of Two-Dimensional Electronic Spectroscopy of Light-Harvesting Complexes

Journal of the American Chemical Society
Francesco SegattaBenedetta Mennucci

Abstract

Nonlinear electronic spectroscopies represent one of the most powerful techniques to study complex multichromophoric architectures. For these systems, in fact, linear spectra are too congested to be used to disentangle the many coupled vibroelectronic processes that are activated. By using a 2D approach, instead, a clear picture can be achieved, but only when the recorded spectra are combined with a proper interpretative model. So far, this has been almost always achieved through parametrized exciton Hamiltonians that necessarily introduce biases and/or arbitrary assumptions. In this study, a first-principles approach is presented that combines accurate quantum chemical descriptions with state-of-the-art models for the environment through the use of atomistic and polarizable embeddings. Slow and fast bath dynamics, along with exciton transport between the pigments, are included. This approach is applied to the 2DES spectroscopy of the Light-Harvesting 2 (LH2) complex of purple bacteria. Simulations are extended over the entire visible-near-infrared spectral region to cover both carotenoid and bacteriochlorophyll signals. Our results provide an accurate description of excitonic properties and relaxation pathways, and give an unp...Continue Reading

References

Mar 23, 2002·Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics·Ana DamjanovićKlaus Schulten
Mar 28, 2002·Biophysical Journal·Sofia GeorgakopoulouGert van der Zwan
Jan 14, 2003·Biophysical Journal·Markus WendlingRienk van Grondelle
Apr 15, 2004·Chemical Reviews·Tomás Polívka, Villy Sundström
Apr 1, 2005·Nature·Tobias BrixnerGraham R Fleming
Aug 17, 2006·Proceedings of the National Academy of Sciences of the United States of America·Donatas ZigmantasGraham R Fleming
Feb 5, 2009·The Journal of Chemical Physics·Martin KleinschmidtStefan Grimme
Jun 10, 2010·Physical Chemistry Chemical Physics : PCCP·Vladimir I Novoderezhkin, Rienk van Grondelle
Jan 29, 2011·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Mihkel PajusaluArvi Freiberg
Jun 4, 2011·The Journal of Physical Chemistry. B·Carsten OlbrichUlrich Kleinekathöfer
Jan 5, 2012·Proceedings of the National Academy of Sciences of the United States of America·Elad Harel, Gregory S Engel
Mar 28, 2013·The Journal of Physical Chemistry. B·Vladimir Novoderezhkin, Rienk van Grondelle
Apr 26, 2014·The Journal of Physical Chemistry. B·Toru Saito, Walter Thiel
Jun 20, 2014·The Journal of Physical Chemistry. B·Olga Rancova, Darius Abramavicius
Aug 26, 2014·The Journal of Physical Chemistry. B·Masahiro HigashiShinji Saito
Oct 17, 2014·The Journal of Physical Chemistry. B·Roel TempelaarJasper Knoester
Jan 3, 2015·The Journal of Physical Chemistry. B·C P van der VegteT L C Jansen
Nov 13, 2015·Journal of Computational Chemistry·Francesco AquilanteRoland Lindh
Jul 14, 2009·Journal of Chemical Theory and Computation·Carles CurutchetBenedetta Mennucci
Jan 23, 2016·Journal of Chemical Theory and Computation·André AndaLuca De Vico
Feb 10, 2016·Scientific Reports·Marco FerrettiRienk van Grondelle
Mar 10, 2016·Chemical Reviews·Carles Curutchet, Benedetta Mennucci
Apr 20, 2016·Annual Review of Physical Chemistry·Mi Kyung LeeDavid F Coker
Jul 19, 2016·Chemical Reviews·Tihana MirkovicGregory D Scholes
Nov 2, 2016·The Journal of Physical Chemistry. B·Clement StrossFrederick R Manby
Nov 2, 2016·The Journal of Physical Chemistry Letters·Riccardo GuareschiClaudia Filippi
Oct 30, 2016·The Journal of Physical Chemistry. B·Lorenzo CupelliniBenedetta Mennucci

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Citations

Mar 27, 2018·Photochemical & Photobiological Sciences : Official Journal of the European Photochemistry Association and the European Society for Photobiology·Daniele LocoBenedetta Mennucci
Apr 28, 2018·Journal of Computational Chemistry·Maxim I KozlovIlya O Glebov
Sep 24, 2019·Faraday Discussions·Javier Segarra-MartíMarco Garavelli
Apr 17, 2020·Photosynthesis Research·Nicoletta LiguoriSebastian Thallmair
Apr 15, 2019·The Journal of Chemical Physics·Matteo CarliPietro Faccioli
Dec 21, 2017·Physical Chemistry Chemical Physics : PCCP·André AndaThorsten Hansen
Jun 9, 2020·The Journal of Chemical Physics·Francesco AquilanteValera Veryazov
Aug 26, 2020·Journal of the American Chemical Society·Irene ContiMarco Garavelli
Sep 10, 2020·The Journal of Physical Chemistry. B·Lorenzo CupelliniJianshu Cao
Aug 7, 2019·Biochimica Et Biophysica Acta. Bioenergetics·Lorenzo CupelliniBenedetta Mennucci
Apr 21, 2021·Physical Chemistry Chemical Physics : PCCP·Sayan MaityUlrich Kleinekathöfer
Dec 16, 2017·Journal of Chemical Theory and Computation·Justin ProvazzaDavid F Coker
Mar 1, 2018·The Journal of Physical Chemistry Letters·Marco SchröterDonatas Zigmantas
Dec 29, 2020·Journal of Chemical Theory and Computation·Justin ProvazzaDavid F Coker
Aug 19, 2020·The Journal of Physical Chemistry Letters·Michael S ChenThomas E Markland
Nov 20, 2018·The Journal of Physical Chemistry Letters·Lorenzo CupelliniBenedetta Mennucci
Jun 28, 2019·The Journal of Physical Chemistry. a·André AndaLuca De Vico
Jul 6, 2019·Chemical Reviews·Francesco SegattaBenedetta Mennucci
Feb 14, 2019·The Journal of Physical Chemistry. B·Amber JainJoseph E Subotnik
Jan 2, 2019·The Journal of Physical Chemistry Letters·Sara C MasseyGregory S Engel
Jun 24, 2020·The Journal of Physical Chemistry. B·Maxim I Kozlov, Vladimir V Poddubnyy
Sep 16, 2021·The Journal of Physical Chemistry. B·Kazuhiro J FujimotoTakeshi Yanai
Nov 30, 2021·Physical Chemistry Chemical Physics : PCCP·Kwang Hyun Cho, Young Min Rhee

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