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The Journal of Chemical Physics

Markovian master equation for a classical particle coupled with arbitrary strength to a harmonic bath

Maxim F. Gelin

Published Dec 3, 2014• 3 citations
Publisher

Abstract

We consider a classical point particle bilinearly coupled to a harmonic bath. Assuming that the evolution of the particle is monitored on a timescale which is longer than the characteristic bath correlation time, we derive the Markovian master equation for the probability density of the particle. The relaxation operator of this master equation is evaluated analytically, without invoking the perturbation theory and the approximation of weak system-bath coupling. When the bath correlation time tends to zero, the Fokker-Planck equation is recovered. For a finite bath correlation time, the relaxation operator contains contributions of all orders in the system-bath coupling.

DOI
10.1063/1.4902438

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We consider a classical point particle bilinearly coupled to a harmonic bath. Assuming that the evolution of the particle is monitored on a timescale which is longer than the characteristic bath correlation time, we derive the Markovian master equation for the probability density of the particle. The relaxation operator of this master equation is evaluated analytically, without invoking the perturbation theory and the approximation of weak system-bath coupling. When the bath correlation time tends to zero, the Fokker-Planck equation is recovered. For a finite bath correlation time, the relaxation operator contains contributions of all orders in the system-bath coupling.
We develop a generalized quantum Fokker-Planck theory in a non-Gaussian-Markovian model bath. The semiclassical bath adopted in this work is charactered by three parameters. One denotes the strength of system-bath coupling and the other two are chosen to interpolate smoothly the solvation dynamics between the long- and short-time regimes. The fluctuation-dissipation relation in this model bath is analyzed in detail. Based on this model bath, we derive two sets of coupled Fokker-Planck equations. These two equation sets are equivalent in the second order of system-bath coupling but different in the higher orders. The corresponding reduced Liouville equation in one set of the Fokker-Planck formulation is characterized by a memory relaxation kernel, while that in the other is by a local-time relaxation tensor. Each resulting set of Fokker-Planck equations involves only the reduced density operator and a series of well-characterized Hilbert-space relaxation operators. The present theory is valid for arbitrary time-dependent Hamiltonians and is applicable to the study of quantum coherence and relaxation in various dynamic systems.
Fourth-order quantum master equations (FQMEs) are derived in both time nonlocal and local forms for a general system Hamiltonian, with new detailed expressions for the fourth-order kernel, where the bath correlation functions are explicitly decoupled from the system superoperators. Further simplifications can be made for the model of linearly coupled harmonic oscillator bath. Consideration of the high temperature Ohmic bath limit leads to a general Markovian FQME with compact forms of time independent superoperators. Two examples of this equation are then considered. For the system of a quantum particle in a continuous potential field, the equation reduces to a known form of the quantum Fokker–Planck equation, except for a fourth-order potential renormalization term that can be neglected only in the weak system-bath interaction regime. For a two-level system with off-diagonal coupling to the bath, fourth-order corrections do not alter the relaxation characteristics of the second-order equation and introduce additional coherence terms in the equations for the off-diagonal elements.
We consider a model of non-Markovian quantum Brownian motion that consists of a harmonic oscillator bilinearly coupled to a thermal bath, both via its position and via its momentum operators. We derive the master equation for such a model, and we solve the equations of motion for a generic Gaussian system state. We then investigate the resulting evolution of the first and second moments for both an Ohmic and a super-Ohmic spectral density. In particular, we show that, irrespective of the specific form of the spectral density, the coupling with the momentum enhances the dissipation experienced by the system, accelerating its relaxation to the equilibrium as well as modifying the asymptotic state of the dynamics. Eventually, we characterize explicitly the non-Markovianity of the evolution using a general criterion which relies on the positivity of the master equation coefficients.
We construct a quantum Markovian master equation for a driven system coupled to a thermal bath. The derivation utilizes an explicit solution of the propagator of the driven system. This enables the validity of the master equation to be extended beyond the adiabatic limit. The nonadiabatic master equation (NAME) is derived employing the weak system-bath coupling limit. The NAME is valid when a separation of timescales exists between the bath dynamics and the external driving. In contrast to the adiabatic master equation, the NAME leads to coupled equations of motion for the population and coherence. We employ the NAME to solve the example of an open driven time-dependent harmonic oscillator. For the harmonic oscillator the NAME predicts the emergence of coherence associated with the dissipation term. As a result of the nonadiabatic driving the thermalization rate is suppressed. The solution is compared with both numerical calculations and the adiabatic master equation.
The Wigner transform of the master equation describing the reduced dynamics of the system, of a harmonic oscillator coupled to an oscillator bath, was obtained by Karrlein and Grabert [Phys. Rev. E 55, 153 (1997)]. It was shown that for some special correlated initial conditions the master equation reduces, in the classical limit, to the corresponding classical Fokker-Planck equation obtained by Adelman [J. Chem Phys. 64, 124 (1976)]. However, for separable initial conditions the Adelman equations were not recovered. We resolve this problem by showing that, for separable initial conditions, the classical Langevin equations are somewhat different from the one considered by Adelman. We obtain the corresponding Fokker-Planck equation and show that they exactly match the classical limit of the evolution of the Wigner function obtained from the master equation for separable initial conditions. We also discuss why thermal initial conditions correspond to Adelman's solution.
The relaxation processes in a quantum system nonlinearly coupled to a harmonic Gaussian-Markovian heat bath are investigated by the quantum Fokker-Planck equation in the hierarchy form. This model describes frequency fluctuations in the quantum system with an arbitrary correlation time and thus bridges the gap between the Brownian oscillator model and the stochastic model by Anderson and Kubo. The effects of the finite correlation time and the system-bath coupling strength are studied for a harmonic model system by numerically integrating the equation of motion. The one-time correlation function of the system coordinate, which is measured in conventional Raman and infrared absorption experiments, already reflects the inhomogeneous character of the relaxation process. The finite correlation time of the frequency fluctuations, however, is directly evident only in the two- and three-time correlation function as probed by multidimensional spectroscopic techniques such as the Raman echo and the fifth-order 2D Raman experiment.