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Tunneling and vibrational relaxation in driven multi-level systems

Michael Thorwart, Milena Grifoni, Peter Hänggi A

Published Dec 6, 1999• 3 citations
OpenAlex

Abstract

We investigate on a unified basis tunneling and vibrational relaxation in driven dissipative multi-stable systems described by their N lowest lying unperturbed levels. By use of the discrete variable representation} we derive a set of coupled non-Markovian master equations. We present analytical treatments that well describe the dynamics as long as the friction strength does not exceed level-broadening amongst neighbouring doublets or the temperature is not too low. This is corroborated by ``ab-initio'' real-time path integral calculations.

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We investigate on a unified basis tunneling and vibrational relaxation in driven dissipative multi-stable systems described by their N lowest lying unperturbed levels. By use of the discrete variable representation} we derive a set of coupled non-Markovian master equations. We present analytical treatments that well describe the dynamics as long as the friction strength does not exceed level-broadening amongst neighbouring doublets or the temperature is not too low. This is corroborated by ``ab-initio'' real-time path integral calculations.
The real-time dynamics of a quantum-mechanical particle in a dissipative double-well potential at finite temperatures is solved ab initio by means of a multisite spin-hopping analysis. Both the macroscopic-quantum-coherence and macroscopic-quantum-tunneling regimes are covered. The theory gives a unified picture of tunneling transport and vibrational relaxation. The analysis is based on the Ohmic-model Hamiltonian [A. O. Caldeira and A. J. Leggett, Ann. Phys. (N.Y.) 149, 374 (1983); R. Zwanzig, J. Stat. Phys. 9, 215 (1973)] or the equivalent ``particle-on-a-string'' model [H. Dekker, Phys. Rev. A 31, 1067 (1985)]. The reduced quantum Liouville equation for the particle is derived and written in the energy representation. The usual truncation to the ground-state doublet of the vibrational ladder is not made. The interdoublet vibrational dynamics considerably simplifies upon coarse-graining and in the harmonic-well approximation. The intradoublet pseudospin dynamics is treated in the ``noninteracting-blip approximation'' [A. J. Leggett et al., Rev. Mod. Phys. 59, 1 (1987)]. The coarse-grained vibrational processes give rise to a Markovian one-step spin hopping between adjacent doublets (or sites). Inter alia ``inhomogeneous broadening'' and ``motional narrowing'' [P. E. Parris and R. Silbey, J. Chem. Phys. 83, 5619 (1985)] are discussed as special cases.
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.
There has been considerable interest recently in the low temperature dynamics of condensed phase tunneling phenomena. In this paper we consider the interplay between quasiparticle transport and vibrational relaxation; the former taking place via tunneling in a double well potential, and the latter occurring due to interactions of the tunneling system with a harmonic bath. Taking the system–bath interactions to be linear in the bath coordinates, and explicitly allowing for a vibrationally excited well, we present a unified treatment of the weak and strong coupling regimes and obtain reduced equations of motion for the tunneling particle position operator. Solutions are obtained for several important limiting cases. In particular, we find that at sufficiently low temperatures, the dynamical behavior strongly resembles that of multisite spin jump model.
We study a driven two-state system interacting with a generic structured environment. We outline the derivation of the time-local microscopic non-Markovian master equation, in the limit of weak coupling between the system and the reservoir, and we derive its analytic solution for general reservoir spectra in the regime of validity of the secular approximation. We also consider the non-Markovian master equation without the secular approximation and study the effect of nonsecular terms on the system dynamics for two classes of reservoir spectra: the Ohmic and the Lorentzian reservoir. Finally, we derive the analytic conditions for complete positivity of the dynamical map, with and without the secular approximation. Interestingly, the complete positivity conditions have a transparent physical interpretation in terms of the characteristic time scales of phase diffusion and relaxation processes.
We study the non-Markovian dynamics of multilevel quantum systems coupled with a bosonic dissipative environment. Based on the known exact quantum-state diffusion (QSD) equations, we propose a systematic approach to derive exact time-convolutionless master equations for multilevel quantum systems. Through a combination of analytical and numerical approaches, we extract the non-Markovian dynamics of quantum interference in different time scales. Also, we demonstrate the evolution of quantum interference in a four-level system controlled by an external electromagnetic field. Our findings are extended to few-body quantum networks, with a universal formalism established.