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The Journal of Chemical Physics

The influence of dissipation on the quantum-classical correspondence: Stability of stochastic trajectories

Maksym Kryvohuz, Jianshu Cao

Published Jun 18, 2009• 18 citations
Publisher

Abstract

The quantum-classical correspondence in the presence of dissipation is studied. The semiclassical expression for the linear response function of an anharmonic system is expressed in a series containing classical stability matrix elements, which can diverge due to the chaotic behavior of stochastic trajectories. The presence of dissipation in most cases removes the divergence of higher-order correction terms, thus suppressing quantum effects and making the system more classical. The regime of system-bath coupling, which makes quantum dynamics completely classical, is obtained in terms of friction, temperature, and anharmonicity. Special cases when bath coupling may lead to enhancement of quantum effects are discussed.

DOI
10.1063/1.3154142

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The quantum-classical correspondence in the presence of dissipation is studied. The semiclassical expression for the linear response function of an anharmonic system is expressed in a series containing classical stability matrix elements, which can diverge due to the chaotic behavior of stochastic trajectories. The presence of dissipation in most cases removes the divergence of higher-order correction terms, thus suppressing quantum effects and making the system more classical. The regime of system-bath coupling, which makes quantum dynamics completely classical, is obtained in terms of friction, temperature, and anharmonicity. Special cases when bath coupling may lead to enhancement of quantum effects are discussed.
The effect of dissipation on the recovery of the classical chaotic dynamics is discussed in the semiclassical regime of the quantum nonintegrable systems. In the classically chaotic Hamiltonian systems, the semiclassical approach breaks down within rather short time scale due to the interference of the wave function. It is shown that the dissipation suppresses the interference and confines the quantum fluctuation around the semiclassical trajectory which is described by the semiclassical Langevin equation. We also show that the semiclassical condition obtained by Schmid is equivalent to the condition for the suppression of interference. The discussion is valid regardless whether the classical motion is chaotic or not and therefore dissipation helps the recovery of the classical dynamics in the chaotic systems.
We develop a method for the determination of the dynamics of dissipative quantum systems in the limit of large number of quanta N , based on the 1/ N -expansion of Heidmann et al. (1985 Opt. Commun. 54 189) and the quantum-classical correspondence. Using this method, we find analytically the dynamics of nonclassical states generation in the higher-order anharmonic dissipative oscillators for an arbitrary temperature of a reservoir. We show that the quantum correction to the classical motion increases with time quadratically up to some maximal value, which is dependent on the degree of nonlinearity and a damping constant, and then it decreases. Similarities and differences with the corresponding behavior of the quantum corrections to the classical motion in the Hamiltonian chaotic systems are discussed. We also compare our results obtained for some limiting cases with the results obtained by using other semiclassical tools and discuss the conditions for validity of our approach.
We discuss the possibility of having "quantum dissipation" due to the interaction with chaotic degrees of freedom. We define the conditions that should be satisfied in order to have a dissipative effect similar to the one due to an interaction with a (many body) bath. We also compare with the case where the environment is modeled by a random matrix model. In the case of interaction with "chaos" we observe a regime where the relaxation process is nonuniversal and reflects the underlaying semiclassical dynamics. As an example we consider a two level system (spin) that interacts with a two-dimensional anharmonic oscillator.
Usually one finds that dissipation tends to make a quantum system more classical in nature. We study the effect of momentum dissipation on a quantum system. The momentum of the particle is coupled bi-linearly to the momenta of a harmonic oscillator heat bath. For a harmonic oscillator system we find that the position and momentum variances for momentum coupling are, respectively, identical to momentum and position variances for spatial friction. This implies that momentum coupling leads to an increase in the fluctuations in position as the temperature is lowered, exactly the opposite of the classical-like localization of the oscillator, found with spatial friction. For a parabolic barrier, momentum coupling causes an increase in the unstable normal mode barrier frequency, as compared to the lowering of the barrier frequency in the presence of purely spatial coupling. This increase in the frequency leads to an enhancement of the thermal tunneling flux, which below the crossover temperature becomes exponentially large. The crossover temperature between tunneling and thermal activation increases with momentum friction so that quantum effects in the escape are relevant at higher temperatures.
The dynamics of a mixed quantum-classical system, in which the classical subsystem interacts with a dissipative bath, is investigated. This description of the dynamics will be appropriate if the details of the bath dynamics are unimportant but its presence plays an important role in the dissipation of energy to the environment. In this dynamical description, which can be simulated employing an ensemble of stochastic surface-hopping trajectories, the strength of the dissipation is controlled by a friction coefficient. We show that if decoherence, whose effects are controlled by the bath friction, is sufficiently rapid, the equation of motion can be reduced to a master equation. Thus, decoherence and the validity of master equation models may be explored as a function of bath friction. We use this framework to study the mechanism of decoherence in a simple model nonadiabatic chemical reaction.
We study the effects of dissipation and decoherence induced on a harmonic oscillator by the coupling to a chaotic system with two degrees of freedom. Using the Feynman-Vernon approach and treating the chaotic system semiclassically, we show that the effects of the low-dimensional chaotic environment are in many ways similar to those produced by thermal baths. The classical correlation and response functions play important roles in both classical and quantum formulations. Our results are qualitatively similar to the high-temperature regime of the Caldeira-Leggett model.