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Updated: May 15, 2026

Generation and Coherent Control of Pulsed Quantum Frequency Combs
Published on: June 8, 2018
How to recover Marcus theory with fewest switches surface hopping: add just a touch of decoherence
Brian R Landry1, Joseph E Subotnik
1Department of Chemistry, University of Pennsylvania, 231 S. 34th Street, Philadelphia, Pennsylvania 19104, USA.
Abstract:
We present a slightly improved version of our augmented fewest switches surface hopping (A-FSSH) algorithm and apply it to the calculation of transition rates between diabatic electronic states within the spin-boson model. We compare A-FSSH rates with (i) Marcus rates from the golden rule, (ii) Tully-style FSSH rates, and (iii) FSSH rates using a simple, intuitive decoherence criterion. We show that unlike FSSH, A-FSSH recovers the correct scaling with diabatic coupling (quadratic in V) as well as the lack of dependence on harmonic frequency ω for small enough values of ω and large enough temperatures.
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