Joel Yuen-Zhou, Jacob J. Krich, Alán Aspuru-Guzik
We report a conceptually straightforward witness that isolates coherent electronic oscillations from their general vibronic counterparts in nonlinear optical spectra of molecular aggregates. The witness is simpler to implement than quantum process tomography, and can be summarized as follows: Coherent oscillations as a function time in broadband pump/broadband probe spectra correspond to electronic coherent oscillations. Oscillations in individual peaks of a rephasing electronic spectrum do not readily yield this conclusion. Our proposal potentially resolves a long-standing controversy on the character of oscillations in ultrafast spectra of photosynthetic light harvesting systems.
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http://arxiv.org/abs/1203.6349
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