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dc.contributor.authorZhao, Yangen
dc.contributor.authorBricker, William P.en
dc.contributor.authorShenai, Prathamesh M.en
dc.contributor.authorGhosh, Avisheken
dc.contributor.authorLiu, Zhengtangen
dc.contributor.authorEnriquez, Miriam Grace M.en
dc.contributor.authorLambrev, Petar H.en
dc.contributor.authorTan, Howe-Siangen
dc.contributor.authorLo, Cynthia S.en
dc.contributor.authorTretiak, Sergeien
dc.contributor.authorFernandez-Alberti, Sebastianen
dc.identifier.citationBricker, W. P., Shenai, P. M., Ghosh, A., Liu, Z., Enriquez, M. G. M., Lambrev, P. H., et al. (2015). Non-radiative relaxation of photoexcited chlorophylls: theoretical and experimental study. Scientific Reports, 5, 13625-.en
dc.description.abstractNonradiative relaxation of high-energy excited states to the lowest excited state in chlorophylls marks the first step in the process of photosynthesis. We perform ultrafast transient absorption spectroscopy measurements, that reveal this internal conversion dynamics to be slightly slower in chlorophyll B than in chlorophyll A. Modeling this process with non-adiabatic excited state molecular dynamics simulations uncovers a critical role played by the different side groups in the two molecules in governing the intramolecular redistribution of excited state wavefunction, leading, in turn, to different time-scales. Even given smaller electron-vibrational couplings compared to common organic conjugated chromophores, these molecules are able to efficiently dissipate about 1 eV of electronic energy into heat on the timescale of around 200 fs. This is achieved via selective participation of specific atomic groups and complex global migration of the wavefunction from the outer to inner ring, which may have important implications for biological light-harvesting function.en
dc.relation.ispartofseriesScientific Reportsen
dc.rightsThis 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
dc.titleNon-radiative relaxation of photoexcited chlorophylls: theoretical and experimental studyen
dc.typeJournal Articleen
dc.contributor.schoolSchool of Materials Science & Engineeringen
dc.contributor.schoolSchool of Physical and Mathematical Sciencesen
dc.description.versionPublished versionen
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