期刊
SCIENTIFIC REPORTS
卷 5, 期 -, 页码 -出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/srep13625
关键词
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资金
- Singapore National Research Foundation through the Competitive Research Programme (CRP) [NRF-CRP5-2009-04]
- U.S. Department of Energy (DOE) Office of Science by Los Alamos National Laboratory [DE-AC52-06NA25396]
- Sandia National Laboratories [DE-AC04-94AL85000]
- Photosynthetic Antenna Research Center (PARC), an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC 0001035]
- Hungarian National Innovation Office
- A*STAR [TET_10-1-2011-0279]
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.
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