Vibrational vs. electronic coherences in 2D spectrum of molecular systems

Abstract

The two-dimensional spectroscopy has recently revealed oscillatory behavior of excitation dynamics in molecular systems. However, in the majority of cases it is strongly debated if excitonic or vibrational wavepackets, or evidences of quantum transport have been observed. In this letter, the method for distinguishing between vibrational and excitonic wavepacket motion is presented, based on the phase and amplitude relationships of oscillations of distinct peaks, which has been revealed using fundamental analysis of two-dimensional spectrum of two representative systems.

References in corpus (3)

• Highly efficient energy excitation transfer in light-harvesting complexes: The fundamental role of noise-assisted transport
• Role of quantum coherence in chromophoric energy transport
• Vibrational wave packet induced oscillations in two-dimensional electronic spectra. I. Experiments

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