An efficient algorithm for capturing quantum effects in classical reactive scattering: application to D + H +3 → H2D+ + H

Literature Information

Publication Date 2022-12-15
DOI 10.1039/D2CP05108G
Impact Factor 3.676
Authors

Matthew Braunstein, Laurent Bonnet


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Abstract

Motivated by a recent semiclassical analysis of chemical reaction thresholds [Bonnet et al., J. Chem. Phys., 2022, 157, 094114], we present an efficient algorithm for including zero-point energy (ZPE) effects in classical reactive scattering. The algorithm is an extension of the quasi-classical trajectory (QCT) Gaussian binning method. We apply it to the astrophysically important D + H+3 reaction, where there are significant quantum effects and where application of other methods is problematic [Braunstein et al., Phys. Chem. Chem. Phys., 2022, 24, 5489]. The rate constants computed with the new, general algorithm closely match recent Ring Polymer Molecular Dynamics (RPMD) [Bulut et al., J. Phys. Chem. A, 2019, 123, 8766] and experimentally derived [Bowen et al., J. Chem. Phys., 2021, 154, 084307] ones spanning ∼4 orders of magnitude from 70 to 1500 K.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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