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Published in

National Academy of Sciences, Proceedings of the National Academy of Sciences, 39(117), p. 24069-24075, 2020

DOI: 10.1073/pnas.2015988117

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Visualizing conical intersection passages via vibronic coherence maps generated by stimulated ultrafast X-ray Raman signals

This paper is made freely available by the publisher.
This paper is made freely available by the publisher.

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Abstract

Significance The capabilities of modern X-ray sources have substantially increased the temporal and spectral resolutions for the observation of elementary molecular events. Theoretically, it has been shown that these unique features can be exploited to probe vibronic coherences that emerge when molecules pass through conical intersections. Here, we demonstrate this technique for the photorelaxation of the RNA-nucleobase uracil after UV excitation. The generated coherence maps reveal the path of the nuclear wavepacket on the excited-state surface in the vicinity of the conical intersection. This information is directly accessible from the spectroscopically recorded signal. Being transferrable to other molecules, these coherence maps will provide detailed visualizations of other nonadiabatic passages in the future.