Tunneling dynamics in dissipative curve-crossing problems

Dmitrii E. Makarov, Nancy Makri

Research output: Contribution to journalArticlepeer-review

Abstract

We have studied the real-time dynamics of dissipative tunneling between two coupled diabatic surfaces. The interplay of tunneling, vibrational relaxation, dephasing, and resonances leads to various regimes of population dynamics, from coherent oscillations between the surfaces to exponential decay described by a rate constant. To describe these phenomena, we exploited recent efficient discretized-path-integral techniques; the two-surface system is treated exactly using a numerically constructed propagator, while the effects of the dissipative environment are incorporated through an influence functional. This procedure results in a low-dimensional integral, which is evaluated by quadrature. Use of a discrete-variable representation (DVR) allows us to replace continuous paths by paths that sample a small set of coordinate points; in particular, the conventional two-level-system approximation is shown to correspond to the limit of two DVR points. The specific features pertinent to nonadiabatic tunneling are discussed.

Original languageEnglish (US)
Pages (from-to)3626-3635
Number of pages10
JournalPhysical Review A
Volume48
Issue number5
DOIs
StatePublished - 1993

ASJC Scopus subject areas

  • Atomic and Molecular Physics, and Optics

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