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Wavepacket interferometry for exciton transfer in molecular dimers

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Abstract

A detailed characterization of the pathways of photo-excitations in the coupled chromophores is needed to better characterize electronic energy transfer, a process important for photosynthetic-light harvesting and vision as well as photographic imaging and optical communication technologies. In order to motivate nonlinear wavepacket interferometry3 experiments on energy-transfer complexes in low-temperature media, we have carried out preliminary calculations on a model system comprising two coupled chromophores whose electronic transition dipole moments have specified (nonparallel) relative and lab-frame orientations. We represent Franck-Condon active nuclear modes by incorporating one internal molecular vibration in each monomer4. Because the energy-transfer matrix element, J, is nonzero selective ultrafast excitation of the donor moiety triggers surface-crossing to the acceptor-excited state yielding dynamical formation of an entangled one-exciton state.

© 2002 Optical Society of America

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