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.
| Original language | English (US) |
|---|---|
| Article number | 22A513 |
| Journal | Journal of Chemical Physics |
| Volume | 137 |
| Issue number | 22 |
| DOIs | |
| State | Published - Dec 14 2012 |
| Externally published | Yes |
All Science Journal Classification (ASJC) codes
- General Physics and Astronomy
- Physical and Theoretical Chemistry