A witness for coherent electronic vs vibronic-only oscillations in ultrafast spectroscopy

作者:Yuen Zhou Joel*; Krich Jacob J; Aspuru Guzik Alan
来源:Journal of Chemical Physics, 2012, 136(23): 234501.
DOI:10.1063/1.4725498

摘要

We report a conceptually straightforward witness that distinguishes coherent electronic oscillations from their vibronic-only counterparts in nonlinear optical spectra of molecular aggregates. Coherent oscillations as a function of waiting time in broadband pump/broadband probe spectra correspond to coherent electronic oscillations in the singly excited manifold. Oscillations in individual peaks of 2D electronic spectra do not necessarily yield this conclusion. Our witness is simpler to implement than quantum process tomography and potentially resolves a long-standing controversy on the character of oscillations in ultrafast spectra of photosynthetic light harvesting systems.

  • 出版日期2012-6-21