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Communication: Vibrational and vibronic coherences in the two dimensional spectroscopy of coupled electron-nuclear motion

Albert, J; Falge, M; Gomez, S; Sola, IR; Hildenbrand, H; Engel, V; (2015) Communication: Vibrational and vibronic coherences in the two dimensional spectroscopy of coupled electron-nuclear motion. The Journal of Chemical Physics , 143 (4) , Article 041102. 10.1063/1.4927396. Green open access

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Abstract

We theoretically investigate the photon-echo spectroscopy of coupled electron-nuclear quantum dynamics. Two situations are treated. In the first case, the Born-Oppenheimer (adiabatic) approximation holds. It is then possible to interpret the two-dimensional (2D) spectra in terms of vibrational motion taking place in different electronic states. In particular, pure vibrational coherences which are related to oscillations in the time-dependent third-order polarization can be identified. This concept fails in the second case, where strong non-adiabatic coupling leads to the breakdown of the Born-Oppenheimer-approximation. Then, the 2D-spectra reveal a complicated vibronic structure and vibrational coherences cannot be disentangled from the electronic motion.

Type: Article
Title: Communication: Vibrational and vibronic coherences in the two dimensional spectroscopy of coupled electron-nuclear motion
Open access status: An open access version is available from UCL Discovery
DOI: 10.1063/1.4927396
Publisher version: https://doi.org/10.1063/1.4927396
Language: English
Additional information: This version is the version of record. For information on re-use, please refer to the publisher’s terms and conditions.
Keywords: Optical fibers, Spectroscopy, Electronic coupling, Born-Oppenheimer approximation, Vibrational states, Adiabatic theorem, Quantum mechanical principles, Potential energy surfaces, Electrostatics, Schrodinger equations
UCL classification: UCL
UCL > Provost and Vice Provost Offices
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10085695
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