A Unified Langevin Framework for Bosonic and Fermionic Dissipation in Nonadiabatic Electrochemical Proton Transfer

We present an influence functional path integral framework for treating the coupled dynamics of solvated proton and electron transfer within a nonequilibrium open system. This method formulates a generalized Langevin equation describing dynamics in systems where proton is simultaneously coupled to fermionic (metal electrons) and bosonic (solvent phonons) reservoirs. It accounts for multiple dissipative channels without relying on phenomenological assumptions. With this scheme, we capture the relaxation of oscillations associated with large quantum zero-point fluctuations when protons are trapped in a harmonic potential. When the proton's translational motion is slow, the dynamics become effectively Markovian. In this regime, dissipation to the electronic reservoir is characterized by a position-dependent electronic friction. Using an effective electronic model Hamiltonian, we demonstrate that electronic friction introduces a sharp, localized resistance when the proton level crosses the Fermi level, effectively delaying the reaction. In contrast, solvent friction arising from assumed Caldeira-Leggett-type coupling, exerts a uniform, position-independent drag. Both mechanisms contribute comparable amounts to the overall energy dissipation. This framework offers a computationally efficient route to simulate complex electrochemical environments involving multiple dissipative baths.

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Publication Details

Journal
Journal of Chemical Theory and Computation
Published
2025-12-04
DOI
https://doi.org/10.1021/acs.jctc.5c01487
Primary Topic
Spectroscopy and Quantum Chemical Studies
Type
article
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article

A Unified Langevin Framework for Bosonic and Fermionic Dissipation in Nonadiabatic Electrochemical Proton Transfer

Elvis F. Arguelles, Osamu Sugino
Journal of Chemical Theory and Computation
Spectroscopy and Quantum Chemical Studies
article

A Unified Langevin Framework for Bosonic and Fermionic Dissipation in Nonadiabatic Electrochemical Proton Transfer

Elvis F. Arguelles, Osamu Sugino
article en

Abstract

We present an influence functional path integral framework for treating the coupled dynamics of solvated proton and electron transfer within a nonequilibrium open system. This method formulates a generalized Langevin equation describing dynamics in systems where proton is simultaneously coupled to fermionic (metal electrons) and bosonic (solvent phonons) reservoirs. It accounts for multiple dissipative channels without relying on phenomenological assumptions. With this scheme, we capture the relaxation of oscillations associated with large quantum zero-point fluctuations when protons are trapped in a harmonic potential. When the proton's translational motion is slow, the dynamics become effectively Markovian. In this regime, dissipation to the electronic reservoir is characterized by a position-dependent electronic friction. Using an effective electronic model Hamiltonian, we demonstrate that electronic friction introduces a sharp, localized resistance when the proton level crosses the Fermi level, effectively delaying the reaction. In contrast, solvent friction arising from assumed Caldeira-Leggett-type coupling, exerts a uniform, position-independent drag. Both mechanisms contribute comparable amounts to the overall energy dissipation. This framework offers a computationally efficient route to simulate complex electrochemical environments involving multiple dissipative baths.

Journal of Chemical Theory and ComputationVol. 21(24)
The University of Tokyo (JP)
Openalex Percentile: Top 70%
Spectroscopy and Quantum Chemical Studies
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A Unified Langevin Framework for Bosonic and Fermionic Dissipation in Nonadiabatic Electrochemical Proton Transfer — Elvis F. Arguelles, Osamu Sugino · Journal of Chemical Theory and Computation (2025) | TGRS Research Map | TGRS