Simulation of the dynamics of vibrationally mediated photodissociation for deuterated pyrrole

Dmitry V Makhov,Mary Cowperthwaite,Sian Adeyemi,Dmitrii V Shalashilin

doi:10.1088/2399-6528/ac4d39

Dmitry V Makhov, Mary Cowperthwaite + Show 2 more

Open Access

https://doi.org/10.1088/2399-6528/ac4d39

Copy DOI

Abstract

The dynamics of photodissociation for vibrationally pre-excited deuterated pyrrole molecules is simulated using ab initio multiple cloning (AIMC) approach. Total kinetic energy release (TKER) spectra and dissociation times are calculated. The results for pyrrole and deuterated pyrrole molecules with and without vibrational pre-excitation are compared. Calculations show that, as expected, the kinetic energy of additional dissociation fragments is lower in deuterated pyrrole and mostly located in the upper-middle part of the TKER spectrum. However, despite lower energy of dissociative bond vibrations, pre-excitation of deuterated pyrrole leads to higher dissociation yield increase than in pyrrole and significantly shortens dissociation time.

Highlights

February 2022Dmitry V Makhov1,2 , Sian Adeyemi, Mary Cowperthwaite and Dmitrii V Shalashilin
The study of ultrafast excited state dynamics is essential to understand many fundamental biochemical processes
We previously demonstrated [23, 33, 34] that simulations using our ab initio multiple cloning (AIMC) approach [35, 36] can reproduce the principal features of experimental total kinetic energy release (TKER) spectra and velocity map images (VMI) for the photodissociation of pyrrole and other heterocyclic molecules, including the isotopic effect for their deuterated isotopologues

Summary

February 2022

Dmitry V Makhov1,2 , Sian Adeyemi, Mary Cowperthwaite and Dmitrii V Shalashilin. The dynamics of photodissociation for vibrationally pre-excited deuterated pyrrole molecules is licence. Simulated using ab initio multiple cloning (AIMC) approach. Any further distribution of this work must maintain spectra and dissociation times are calculated. The results for pyrrole and deuterated pyrrole molecules attribution to the with and without vibrational pre-excitation are compared. Calculations show that, as expected, the author(s) and the title of the work, journal citation kinetic energy of additional dissociation fragments is lower in deuterated pyrrole and mostly located and DOI. In the upper-middle part of the TKER spectrum. Despite lower energy of dissociative bond vibrations, pre-excitation of deuterated pyrrole leads to higher dissociation yield increase than in pyrrole and significantly shortens dissociation time

Introduction

Theory

Computational details

Results and discussion

Conclusion