The protein environment in photosynthetic light harvesting complexes serves to hold the chromophores in strict geometric alignments, which permits sufficiently strong excitonic coupling that excitations are delocalized over multiple chromophores.  The electronic coupling between these pigments leads to vibronic coupling with shared vibrational modes such that motion of these modes affects multiple electronic states.  Data will be presented that shows that this motion appears to have some surprising character in that all seven strongly coupled excitons in the Fenna-Matthews-Olson complex show similar spectral motion and that motion of an unpopulated excited state shows sympathetic, driven spectral motion.  This data challenges our typical pictures of energy transfer that are built based on random spectral diffusion and independent bath modes.

Ultrafast spectroscopy of synchronized and correlated excited state motions in the presence of spectral diffusion

256th National Meeting (2018)

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