Please use this identifier to cite or link to this item: https://hdl.handle.net/10356/103527
Title: Non-radiative relaxation of photoexcited chlorophylls: theoretical and experimental study
Authors: Zhao, Yang
Bricker, William P.
Shenai, Prathamesh M.
Ghosh, Avishek
Liu, Zhengtang
Enriquez, Miriam Grace M.
Lambrev, Petar H.
Tan, Howe-Siang
Lo, Cynthia S.
Tretiak, Sergei
Fernandez-Alberti, Sebastian
Issue Date: 2015
Source: Bricker, 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-.
Series/Report no.: Scientific Reports
Abstract: Nonradiative 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.
URI: https://hdl.handle.net/10356/103527
http://hdl.handle.net/10220/38764
ISSN: 2045-2322
DOI: 10.1038/srep13625
Rights: 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/
Fulltext Permission: open
Fulltext Availability: With Fulltext
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