Vibronic Dynamics of Photodissociating ICN from Simulations of Ultrafast X‐Ray Absorption Spectroscopy

• Published in: Angewandte Chemie International Edition Vol. 59; no. 45; pp. 20044 - 20048
• Main Authors: Morzan, Uriel N., Videla, Pablo E., Soley, Micheline B., Nibbering, Erik T. J., Batista, Victor S.
• Format: Journal Article
• Language: English
• Published: Germany Wiley Subscription Services, Inc 02.11.2020; John Wiley and Sons Inc
• Edition: International ed. in English
• Subjects: Absorption spectroscopy; ICN; Information processing; Photochemicals; Photodissociation; pump–probe spectroscopy; quantum dynamics; Spectra; Spectrum analysis; time-resolved X-ray spectroscopy; Transient response; ultrafast photochemistry; Wave packets; ultrafast photochemistry; ICN; pump-probe spectroscopy; quantum dynamics; time-resolved X-ray spectroscopy
• ISSN: 1433-7851; 1521-3773; 1521-3773
• DOI: 10.1002/anie.202007192

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. Ultrafast UV‐pump/soft‐X‐ray‐probe spectroscopy provides detailed information about dynamical photochemical processes with ultrafast resolution and atomic specificity. Here, the photodissociation of ICN in the 1Π1 excited state is studied. 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.