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Vibronic Dynamics of Photodissociating ICN from Simulations of Ultrafast X-Ray Absorption Spectroscopy |
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| Authors: | Dr Uriel N Morzan Dr Pablo E Videla Dr Micheline B Soley Dr Erik T J Nibbering Prof Victor S Batista |
| Institution: | 1. Condensed Matter Section, The Abdus Salam International Center for Theoretical Physics, Strada Costiera 11, 34151 Trieste, Italy;2. Department of Chemistry, Yale University, P.O. Box 208107, New Haven, CT, 06520-8107 USA;3. Department of Chemistry, Yale University, P.O. Box 208107, New Haven, CT, 06520-8107 USA
Department of Chemistry and Chemical Biology, Harvard University, 12 Oxford Street, Cambridge, MA, 02138 USA Yale Quantum Institute, Yale University, P.O. Box 208334, New Haven, CT, 06520-8263 USA These authors contributed equally to this work.;4. Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy, Max Born Strasse 2A, 12489 Berlin, Germany |
| Abstract: | Ultrafast UV-pump/soft-X-ray-probe spectroscopy is a subject of great interest since it can provide detailed information about dynamical photochemical processes with ultrafast resolution and atomic specificity. Here, we focus on the photodissociation of ICN in the 1Π1 excited state, with emphasis on the transient response in the soft-X-ray spectral region as described by the ab initio spectral lineshape averaged over the nuclear wavepacket probability density. We find that the carbon K-edge spectral region reveals a rich transient response that provides direct insights into the dynamics of frontier orbitals during the I−CN bond cleavage process. The simulated UV-pump/soft-X-ray-probe spectra exhibit detailed dynamical information, including a time-domain signature for coherent vibration associated with the photogenerated CN fragment. |
| Keywords: | ICN pump–probe spectroscopy quantum dynamics time-resolved X-ray spectroscopy ultrafast photochemistry |