Abstract
We discuss utilization of kinetic schemes for description of open interacting systems, focusing on vibrational energy relaxation for an oscillator coupled to a nonequilibirum electronic bath. Standard kinetic equations with constant rate coefficients are obtained under the assumption of time scale separation between the system and bath, with the bath dynamics much faster than that of the system of interest. This assumption may break down in certain limits, and we show that ignoring this may lead to qualitatively wrong predictions. Connection with more general, nonequilibrium Green's function (NEGF) analysis is demonstrated. Our considerations are illustrated within generic molecular junction models with electron-vibration coupling.
| Original language | English |
|---|---|
| Pages (from-to) | 4886-4892 |
| Number of pages | 7 |
| Journal | Journal of Physical Chemistry Letters |
| Volume | 9 |
| Issue number | 17 |
| DOIs | |
| State | Published - 6 Sep 2018 |
ASJC Scopus subject areas
- General Materials Science
- Physical and Theoretical Chemistry
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