The remarkable efficiency of photosynthetic energy transfer processes has been a mystery for over 75 years.  Recent two-dimensional (2D) spectroscopy experiments have found signatures from a coherence of unexpectedly large amplitude that persists for longer than the apparent energy transfer timescale. We have recently shown that intramolecular vibrations shared across pigments can drive electronic energy transfer beyond the Born-Oppenheimer framework developed by Forster. Such shared vibrations on the ground electronic state of the antenna, in which no pigments are electronically excited, generate all of the reported 2D signatures and their properties indicate some new design principles for light harvesting based on vibrational-electronic resonance. We have computationally studied this mechanism to explore how it can be used to control energy transfer and will discuss these results.

Harnessing shared vibrations to control energy transfer

253rd National Meeting (2017)

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.