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The initial energy transfer in photosynthesis occurs between thelight-harvesting pigments and on ultrafast timescales. We analyze thecarotenoid to bacteriochlorophyll energy transfer in LH2 Marichromatiumpurpuratum as well as in an artificial light-harvesting dyad system by usingtransient grating and two-dimensional electronic spectroscopy with 10 fs timeresolution. We find that F\"orster-type models reproduce the experimentallyobserved 60 fs transfer times, but overestimate coupling constants, which leadsto a disagreement with both linear absorption and electronic 2D-spectra. Weshow that a vibronic model, which treats carotenoid vibrations on bothelectronic ground and excited state as part of the system's Hamiltonian,reproduces all measured quantities. Importantly, the vibronic model presentedhere can explain the fast energy transfer rates with only moderate couplingconstants, which are in agreement with structure based calculations.Counterintuitively, the vibrational levels on the carotenoid electronic groundstate play a central role in the excited state population transfer tobacteriochlorophyll as the resonance between the donor-acceptor energy gap andvibrational ground state energies is the physical basis of the ultrafast energytransfer rates in these systems.

Vibronic coupling explains the ultrafast carotenoid-to-bacteriochlorophyll energy transfer in natural and artificial light harvesters