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We report a conceptually straightforward witness that isolates coherentelectronic oscillations from their vibronic counterparts in nonlinear opticalspectra of molecular aggregates: Coherent oscillations as a function of waitingtime in broadband pump/broadband probe spectra correspond to coherentelectronic oscillations. Oscillations in individual peaks of 2D electronicspectra do not necessarily yield this conclusion. Our witness is simpler toimplement than quantum process tomography and potentially resolves along-standing controversy on the character of oscillations in ultrafast spectraof photosynthetic light harvesting systems.

A witness for coherent electronic oscillations in ultrafast spectroscopy