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Issue 5, 2015
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Ab initio multiple cloning simulations of pyrrole photodissociation: TKER spectra and velocity map imaging

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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.

Graphical abstract: Ab initio multiple cloning simulations of pyrrole photodissociation: TKER spectra and velocity map imaging

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The article was received on 09 Oct 2014, accepted on 09 Dec 2014 and first published on 11 Dec 2014


Article type: Paper
DOI: 10.1039/C4CP04571H
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Phys. Chem. Chem. Phys., 2015,17, 3316-3325
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    Ab initio multiple cloning simulations of pyrrole photodissociation: TKER spectra and velocity map imaging

    D. V. Makhov, K. Saita, T. J. Martinez and D. V. Shalashilin, Phys. Chem. Chem. Phys., 2015, 17, 3316
    DOI: 10.1039/C4CP04571H

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