Two-Dimensional Electronic Spectroscopy Reveals Ultrafast Downhill Energy Transfer in Photosystem I Trimers of the Cyanobacterium Thermosynechococcus elongatus.

Two-dimensional electronic spectroscopy (2DES) was used to investigate the ultrafast energy-transfer dynamics of trimeric photosystem I of the cyanobacterium Thermosynechococcus elongatus. We demonstrate the ability of 2DES to resolve dynamics in a large pigment-protein complex containing ∼300 chromophores with both high frequency and time resolution. Monitoring the waiting-time-dependent changes of the line shape of the inhomogeneously broadened Qy(0-0) transition, we directly observe downhill energy equilibration on the 50 fs time scale.