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We propose a new quantum transition-state theory for calculating Fermi's golden-rule rates in complex multidimensional systems. This method is able to account for the nuclear quantum effects of delocalization, zero-point energy and…

Chemical Physics · Physics 2019-03-27 Manish J. Thapa , Wei Fang , Jeremy O. Richardson

Fermi's golden rule defines the transition rate between weakly coupled states and can thus be used to describe a multitude of molecular processes including electron-transfer reactions and light-matter interaction. However, it can only be…

Chemical Physics · Physics 2020-03-03 Eric R. Heller , Jeremy O. Richardson

Starting from a general molecular Hamiltonian expressed in the basis of adiabatic electronic and nuclear position states, where a compact and complete expression for nonadiabatic derivative coupling (NDC) Hamiltonian term is obtained, we…

Quantum Physics · Physics 2026-01-01 Seogjoo J. Jang , Byeong Ki Min , Young Min Rhee

Fermi's golden rule describes the leading-order behaviour of the reaction rate as a function of the diabatic coupling. Its asymptotic $(\hbar \rightarrow 0)$ limit is the semiclassical golden-rule instanton rate theory, which rigorously…

Chemical Physics · Physics 2022-05-18 George Trenins , Jeremy O. Richardson

We present a simple interpolation formula for the rate of an electron transfer reaction as a function of the electronic coupling strength. The formula only requires the calculation of Fermi Golden Rule and Born-Oppenheimer rates and so can…

Chemical Physics · Physics 2019-09-24 Joseph E. Lawrence , Theo Fletcher , Lachlan P. Lindoy , David E. Manolopoulos

The Marcus theory expression for the rate of non-adiabatic electron transfer is widely used across a range of physical conditions. Although Marcus theory defines the reorganization energy classically, here we show that the reorganization…

Quantum Physics · Physics 2026-04-02 Ethan Abraham , Junghyun Yoon , Troy Van Voorhis , Martin Z. Bazant

With the rapid development of nanophotonics and cavity quantum electrodynamics, there has been growing interest in how confined electromagnetic fields modify fundamental molecular processes such as electron transfer. In this paper, we…

Chemical Physics · Physics 2026-04-20 Wenxiang Ying , Abraham Nitzan

Fermi's Golden Rule (FGR) is one of the most impactful formulas in quantum mechanics, providing a link between easy-to-measure observables - such as transition rates - and fundamental microscopic properties - such as density of states or…

The Nonequilibrium Fermi's Golden Rule (NE-FGR) provides a convenient theoretical framework for calculating the charge transfer rate between a photoexcited bright donor electronic state and a dark acceptor electronic state, when the nuclear…

Quantum Physics · Physics 2025-09-17 Pouya Khazaei , Eitan Geva

Non-adiabatic decay rates for a radio-frequency dressed magnetic trap are calculated using Fermi's Golden Rule: that is, we examine the probability for a single atom to make transitions out of the dressed trap and into a continuum in the…

Atomic Physics · Physics 2017-09-06 Kathryn A Burrows , Barry M Garraway , Hélène Perrin

A novel and readily understandable derivation of the Golden Rule of time dependent perturbation theory is presented. The derivation is based on adiabatic turning on of the perturbation as used, for instance, in some formal developments of…

Quantum Physics · Physics 2020-06-24 M G Burt

Many reactions in chemistry and biology involve multiple electronic states, rendering them nonadiabatic in nature. These reactions can be formally described using Fermi's golden rule (FGR) in the weak-coupling limit. Nonadiabatic instanton…

Chemical Physics · Physics 2025-10-22 Ziyan Ye , Eric R. Heller , Dong H. Zhang , Jeremy O. Richardson , Wei Fang

We present a real-time path integral theory for the rate of electron transfer reactions. Using graph theoretic techniques, the dynamics is expressed in a formally exact way as a set of integral equations. With a simple approximation for the…

chem-ph · Physics 2009-10-28 Juergen T. Stockburger , C. H. Mak

We present a Gedankenexperiment that leads to a violation of detailed balance if quantum mechanical transition probabilities are treated in the usual way by applying Fermi's "golden rule". This Gedankenexperiment introduces a collection of…

Quantum Physics · Physics 2020-09-21 Daniel Braak , Jochen Mannhart

There is currently much interest in the development of improved trajectory-based methods for the simulation of nonadiabatic processes in complex systems. An important goal for such methods is the accurate calculation of the rate constant…

Chemical Physics · Physics 2014-09-04 Jeremy O. Richardson , Michael Thoss

We present a state-space-based path integral method to calculate the rate of electron transfer (ET) in multi-state, multi-electron condensed-phase processes. We employ an exact path integral in discrete electronic states and continuous…

Chemical Physics · Physics 2016-06-07 Jessica Ryan Duke , Nandini Ananth

We evaluate various analytical models for the electron-ion energy transfer and compare the results to data from molecular dynamics (MD) simulations. The models tested includes energy transfer via strong binary collisions, Landau-Spitzer…

Plasma Physics · Physics 2014-03-05 J. Vorberger , D. O. Gericke

Constructing an accurate approximation to nonadiabatic rate theory which is valid for arbitrary values of the electronic coupling has been a long-standing challenge in theoretical chemistry. Ring-polymer instanton theories offer a very…

Chemical Physics · Physics 2025-05-09 Rhiannon A. Zarotiadis , Joseph E. Lawrence , Jeremy O. Richardson

We examine electron transfer between two quantum states in the presence of a dissipative environment represented as a set of independent harmonic oscillators. For this simple model, the Marcus transfer rates can be derived and we show that…

Mesoscale and Nanoscale Physics · Physics 2013-06-11 Lev Mourokh , Seth Lloyd

We study nonadiabatic electron transfer within the biased spin-boson model. We calculate the incoherent transfer rate in analytic form at all temperatures for a power law form of the spectral density of the solvent coupling. In the Ohmic…

Statistical Mechanics · Physics 2009-10-31 G. Lang , E. Paladino , U. Weiss
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