Makhov, DV orcid.org/0000-0003-1795-3820, Saita, K orcid.org/0000-0001-7705-5833, Martinez, TJ orcid.org/0000-0002-4798-8947 et al. (1 more author) (2015) Ab initio multiple cloning simulations of pyrrole photodissociation: TKER spectra and velocity map imaging. Physical Chemistry Chemical Physics, 17 (5). pp. 3316-3325. ISSN 1463-9076
Abstract
We report a detailed computational simulation of the photodissociation of pyrrole using the ab initio Multiple Cloning (AIMC) method implemented within MOLPRO. The efficiency of the AIMC implementation, employing train basis sets, linear approximation for matrix elements, and Ehrenfest configuration cloning, allows us to accumulate significant statistics. We calculate and analyze the total kinetic energy release (TKER) spectrum and Velocity Map Imaging (VMI) of pyrrole and compare the results directly with experimental measurements. Both the TKER spectrum and the structure of the velocity map image (VMI) are well reproduced. Previously, it has been assumed that the isotropic component of the VMI arises from long time statistical dissociation. Instead, our simulations suggest that ultrafast dynamics contributes significantly to both low and high energy portions of the TKER spectrum.
Metadata
Item Type: | Article |
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Authors/Creators: |
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Copyright, Publisher and Additional Information: | This journal is © the Owner Societies 2015. This is an open access article licensed under a Creative Commons Attribution 3.0 Unported Licence. http://creativecommons.org/licenses/by/3.0/ |
Dates: |
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Institution: | The University of Leeds |
Academic Units: | The University of Leeds > Faculty of Engineering & Physical Sciences (Leeds) > School of Chemistry (Leeds) > Physical Chemistry (Leeds) The University of Leeds > Faculty of Engineering & Physical Sciences (Leeds) |
Depositing User: | Symplectic Publications |
Date Deposited: | 30 Sep 2015 15:32 |
Last Modified: | 17 Dec 2024 11:12 |
Published Version: | http://dx.doi.org/10.1039/c4cp04571h |
Status: | Published |
Publisher: | Royal Society of Chemistry |
Identification Number: | 10.1039/c4cp04571h |
Related URLs: | |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:88794 |