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Updated: Aug 9, 2026

Analyzing Melts and Fluids from Ab Initio Molecular Dynamics Simulations with the UMD Package
Published on: September 17, 2021
Connecting chemical dynamics in gases and liquids
Christopher G Elles1, F Fleming Crim
1Department of Chemistry, University of Southern California, Los Angeles, California 90089, USA. elles@anl.gov
Abstract:
Modern ultrafast spectroscopic techniques provide new opportunities to study chemical reaction dynamics in liquids and hold the possibility of obtaining much of the same detailed information available in gases. Vibrational energy transfer studies are the most advanced of the investigations and demonstrate that it is possible to observe state-specific pathways of energy flow within a vibrationally excited molecule (intramolecular vibrational relaxation) and into the surrounding solvent molecules (intermolecular energy transfer). Energy transfer in liquids and gases share many common aspects, but the presence of the solvent also alters the relaxation in both obvious and subtle ways. Photodissociation is amenable to similarly detailed study in liquids, and there are informative new measurements. Bimolecular reactions have received the least attention in state-resolved measurements in liquids, but the means to carry them much further now exist. Studying photodissociation and bimolecular reaction of molecules prepared with initial vibrational excitation in liquids is a realistic, but challenging, goal.
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