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Abstract: We introduce a framework to investigate ab-initio the dynamics of rarethermally activated reactions. The electronic degrees of freedom are describedat the quantum-mechanical level in the Born-Oppenheimer approximation, whilethe nuclear degrees of freedom are coupled to a thermal bath, through aLangevin equation. This method is based on the path integral representation forthe stochastic dynamics and yields the time evolution of both nuclear andelectronic degrees of freedom, along the most probable reaction pathways,without spending computational time to explore metastable states. This approachis very efficient and allows to study thermally activated reactions whichcannot be simulated using ab-initio molecular dynamics techniques. As a firstillustrative application, we characterize the dominant pathway in thecyclobutene to butadiene reaction.



Author: S. a Beccara, G. Garberoglio, P. Faccioli, F. Pederiva

Source: https://arxiv.org/







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