Resolving vibrational from electronic coherences in two-dimensional electronic spectroscopy: The role of the laser spectrum

Franco Valduga De Almeida Camargo, Lena Grimmelsmann, Harry L. Anderson, Stephen R. Meech, Ismael A. Heisler

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Abstract

The observation of coherent quantum effects in photosynthetic light-harvesting complexes prompted the question whether quantum coherence could be exploited to improve the efficiency in new energy materials. The detailed characterization of coherent effects relies on sensitive methods such as two-dimensional electronic spectroscopy (2D-ES). However, the interpretation of the results produced by 2D-ES is challenging due to the many possible couplings present in complex molecular structures. In this work, we demonstrate how the laser spectral profile can induce electronic coherence-like signals in monomeric chromophores, potentially leading to data misinterpretation. We argue that the laser spectrum acts as a filter for certain coherence pathways and thus propose a general method to differentiate vibrational from electronic coherences.
Original languageEnglish
Article number033001
JournalPhysical Review Letters
Volume118
Issue number3
DOIs
Publication statusPublished - 20 Jan 2017

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