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Natural and artificial light harvesting processes have recently gained newinterest. Signatures of long lasting coherence in spectroscopic signals ofbiological systems have been repeatedly observed, albeit their origin is amatter of ongoing debate, as it is unclear how the loss of coherence due tointeraction with the noisy environments in such systems is averted. Here wereport experimental and theoretical verification of coherentexciton-vibrational (vibronic) coupling as the origin of long-lasting coherencein an artificial light harvester, a molecular J-aggregate. In thismacroscopically aligned tubular system, polarization controlled 2D spectroscopydelivers an uncongested and specific optical response as an ideal foundationfor an in-depth theoretical description. We derive analytical expressions thatshow under which general conditions vibronic coupling leads to prolongedexcited-state coherence.

Vibronic origin of long-lived coherence in an artificial molecular light harvester