Probing Conical Intersection in the Multipathway Isomerization of CHCl Using Coulomb Explosion.

J Phys Chem Lett

State Key Laboratory for Mesoscopic Physics and Center for Nano-optoelectronics, School of Physics, Peking University, Beijing 100871, China.

Published: March 2024

AI Article Synopsis

  • The study examines ultrafast isomerization in photoexcited CHCl molecules, focusing on how different electronic states interact non-adiabatically.
  • Using pump-probe Coulomb explosion imaging, the researchers found that isomerization occurs through multiple pathways, with distinct patterns observed in the kinetic energy release spectra.
  • The findings reveal that the strong laser field not only drives isomerization but also influences coherent vibrational dynamics, leading to concurrent reactions in intermediate states.

Article Abstract

Ubiquitous ultrafast isomerization is paramount in photoexcited molecules, in which non-adiabatic coupling among multiple electronic states can occur. We use the pump-probe Coulomb explosion imaging method to study the isomerization of CHCl molecules. We find that the isomerization under our strong field pump-probe scheme proceeds along multiple pathways, which are encoded in several distinct branches of the time-resolved kinetic energy release spectra for the CH+HCl Coulomb explosion channel. Apart from the isomerized dissociative pathway in neutral and cationic excited states, the pump laser can also induce coherent vibrational dynamics in two coupled intermediate states and set up the initial conditions for the two concurrently proceeding isomerization pathways. The isomerization of CHCl provides an intriguing example of a chemical reaction consisting of multiple pathways and non-adiabatic dynamics.

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http://dx.doi.org/10.1021/acs.jpclett.3c03404DOI Listing

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