Toward fully quantum modelling of ultrafast photodissociation imaging experiments. Treating tunnelling in the ab initio multiple cloning approach

Dmitry V Makhov; Todd J Martinez; Dmitrii V Shalashilin

doi:10.1039/c6fd00073h

Toward fully quantum modelling of ultrafast photodissociation imaging experiments. Treating tunnelling in the ab initio multiple cloning approach

Faraday Discuss. 2016 Dec 16:194:81-94. doi: 10.1039/c6fd00073h.

Authors

Dmitry V Makhov¹, Todd J Martinez², Dmitrii V Shalashilin¹

Affiliations

¹ School of Chemistry, University of Leeds, Leeds, LS2 9JT, UK. [email protected] [email protected].
² Department of Chemistry, Stanford University, Stanford, CA 94305, USA.

PMID: 27711808
DOI: 10.1039/c6fd00073h

Abstract

We present an account of our recent effort to improve simulation of the photodissociation of small heteroaromatic molecules using the Ab Initio Multiple Cloning (AIMC) algorithm. The ultimate goal is to create a quantitative and converged technique for fully quantum simulations which treats both electrons and nuclei on a fully quantum level. We calculate and analyse the total kinetic energy release (TKER) spectra and Velocity Map Images (VMI), and compare the results directly with experimental measurements. In this work, we perform new extensive calculations using an improved AIMC algorithm that now takes into account the tunnelling of hydrogen atoms. This can play an extremely important role in photodissociation dynamics.

Publication types

Research Support, Non-U.S. Gov't