| Autor: |
Litman, Y., Pós, E. S., Box, C. L., Martinazzo, R., Maurer, R. J., Rossi, M. |
| Rok vydání: |
2022 |
| Předmět: |
|
| Druh dokumentu: |
Working Paper |
| DOI: |
10.1063/5.0088400 |
| Popis: |
In part I, we presented the ring-polymer instanton with explicit friction (RPI-EF) method and showed how it can be connected to the \textit{ab initio} electronic friction formalism. This framework allows the calculation of tunneling reaction rates that incorporate the quantum nature of the nuclei and certain types of non-adiabatic effects (NAEs) present in metals. In this second part, we analyze the performance of RPI-EF on model potentials and apply it to realistic systems. For a 1D double-well model, we benchmark the method against numerically exact results obtained from multi-layer multi-configuration time-dependent Hartree calculations. We demonstrate that RPI-EF is accurate for medium and high friction strengths and less accurate for extremely low friction values. We also show quantitatively how the inclusion of NAEs lowers the cross-over temperature into the deep tunneling regime, reduces the tunneling rates, and in certain regimes, steers the quantum dynamics by modifying the tunneling pathways. As a showcase of the efficiency of this method, we present a study of hydrogen and deuterium hopping between neighboring interstitial sites in selected bulk metals. The results show that multidimensional vibrational coupling and nuclear quantum effects have a larger impact than NAEs on the tunneling rates of diffusion in metals. Together with part I, these results advance the calculations of dissipative tunneling rates from first principles. |
| Databáze: |
arXiv |
| Externí odkaz: |
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