Abstract
Fast and efficient energy transfer in photosynthetic antennas supports all life on earth. Nonadiabatic energy transfer drives unusual vibrations through tight coupling with electronic motion. Polarization dependent vibrational motion drives polarization independent femtosecond energy transfer.
Highlights
Photosynthesis supports essentially all life on earth
Light is harvested by antennas containing thousands of light absorbing pigment molecules and transferred to reaction centers, which initiate a series of reactions that store energy by synthesizing high energy molecules
The energy transfer reaches a maximum at about 600 fs, when the electronic character is that of the acceptor A and switches sign from |A> to – |A> as the vibrational wavepacket oscillates from side to side with each vibrational half period
Summary
Photosynthesis supports essentially all life on earth. Light is harvested by antennas containing thousands of light absorbing pigment molecules and transferred to reaction centers, which initiate a series of reactions that store energy by synthesizing high energy molecules. Energy transfer[1] and the primary charge separation[2, 3] are ultrafast and extraordinarily efficient, inspiring many investigations of their mechanism. Two-dimensional spectroscopy has revealed unusual quantum beat signatures for both processes,[4] which were initially hypothesized to arise from protein protection of electronic coherence. Recent experiments[5] support an alternative mechanism[1] in which vibrations that are delocalized over more than one pigment are amplified by coupling to electronic motion. We report unusual aspects of such electronically amplified vibrations
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