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  • 标题:Electronic resonance with anticorrelated pigment vibrations drives photosynthetic energy transfer outside the adiabatic framework
  • 本地全文:下载
  • 作者:Vivek Tiwari ; William K. Peters ; David M. Jonas
  • 期刊名称:Proceedings of the National Academy of Sciences
  • 印刷版ISSN:0027-8424
  • 电子版ISSN:1091-6490
  • 出版年度:2013
  • 卷号:110
  • 期号:4
  • 页码:1203-1208
  • DOI:10.1073/pnas.1211157110
  • 语种:English
  • 出版社:The National Academy of Sciences of the United States of America
  • 摘要:The delocalized, anticorrelated component of pigment vibrations can drive nonadiabatic electronic energy transfer in photosynthetic light-harvesting antennas. In femtosecond experiments, this energy transfer mechanism leads to excitation of delocalized, anticorrelated vibrational wavepackets on the ground electronic state that exhibit not only 2D spectroscopic signatures attributed to electronic coherence and oscillatory quantum energy transport but also a cross-peak asymmetry not previously explained by theory. A number of antennas have electronic energy gaps matching a pigment vibrational frequency with a small vibrational coordinate change on electronic excitation. Such photosynthetic energy transfer steps resemble molecular internal conversion through a nested intermolecular funnel.
  • 关键词:2D spectroscopy ; exciton ; Förster resonance energy transfer
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