期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 17, 期 5, 页码 3316-3325出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c4cp04571h
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资金
- EPSRC [EP/I014500/1, EP/J001481/1]
- NSF [CHE-11-24515]
- Engineering and Physical Sciences Research Council [EP/J001481/1, EP/I014500/1] Funding Source: researchfish
- Division Of Chemistry [1124515] Funding Source: National Science Foundation
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.
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