Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 110, Issue 4, Pages 1203-1208Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1211157110
Keywords
2D spectroscopy; exciton; Forster resonance energy transfer
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Funding
- National Science Foundation Grant [CHE-1112365, CNS-0821794]
- University of Colorado at Boulder
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1112365] Funding Source: National Science Foundation
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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.
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