The quantum Fokker-Planck equation is derived for a system nonlinearly coupled to a harmonic oscillator bath. The system-bath interaction is assumed to be linear in the bath coordinates but quadratic in the system coordinate. The relaxation induced dynamics of a harmonic system are investigated by simulating the higher-order correlation functions of the Raman polarizability and the dipole moment, which represent the nonlinear optical responses of Raman or infrared spectroscopy. The 5th-order Raman response shows that, in addition to the frequency fluctuations induced by the bath, higher-order energy transfer between the system and bath plays a role. The nonlinearity of the system-bath interaction yields also an interesting feature in the 7th-order Raman echo or the 3rd-order infrared photon echo response: The calculations predict a finite signal for the case of a harmonic potential and a linear coordinate dependence of the polarizability or dipole while for linear system-bath coupling this response vanishes completely due to destructive interference of different Liouville space pathways.
Vibrational relaxation of a harmonic oscillator nonlinearly coupled to a heat bath is investigated by the Gaussian–Markovian quantum Fokker–Planck equation approach. The system–bath interaction is assumed to be linear in the bath coordinate, but linear plus square in the system coordinate modeling the elastic and inelastic relaxation mechanisms. Interplay of the two relaxation processes induced by the linear–linear and square–linear interactions in Raman or infrared spectra is discussed for various system–bath couplings, temperatures, and correlation times for the bath fluctuations. The one-quantum coherence state created through the interaction with the pump laser pulse relaxes through different pathways in accordance with the mechanisms of the system–bath interactions. Relations between the present theory, Redfield theory, and stochastic theory are also discussed.
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.
Building upon the work of Hu, Paz, and Zhang [1,2] on open quantum systems we consider the quantum Brownian motion (QBM) model with one oscillator (position variable
x) as the system, {\it nonlinearly} coupled to an environment of
N harmonic oscillators (with mass
mn, natural frequency
ωn, position
qn and momentum
pn variables) in the form
∑n(vn1(x)qnk+vn2(x)pnl) where
k,l are integers (the present work only considers the
k=l=2 cases). The vertex functions $v_{n1}, v_{n2} $ are of the form
vn1=λCn1f(x),vn2(x)=−λCn2mn−2ωn−2f(x) where
Cn1,2 are the coupling constants with the
nth oscillator,
f(x) is any arbitrary function of
x, and
λ is a dimensionless constant. Employing the closed-time-path formalism the influence action
SIF is calculated using a perturbative expansion in
λ. It is possible to identify the terms in
SIF quadratic or higher in
Δ(s)≡f(x+(s))−f(x−(s)) to constitute the noise kernel, while terms linear in
Δ to that of the dissipation kernel. The non-Gaussian noise kernel gives rise to non-zero three-point correlation function of the corresponding stochastic force. The pathway presented here should be useful for the exploration of \textit{non-Gaussian properties of systems nonlinearly coupled with their environments}; examples in early universe cosmology and in quantum optomechanics (QOM) are mentioned. A modified fluctuation-dissipation relation (FDR) is also established, which ensures the consistency of the model and the accuracy of results even at higher perturbative orders. Another result of significance is the derivation of a nonlinear Langevin equation which is expected to be useful for many open quantum system applications.
We analyze the behavior of a damped quantum harmonic oscillator immersed in a heat bath with a nonlinear coupling. For this purpose, we construct a generalized master equation (GME) for the reduced density of the oscillator. We specialize the results for a quadratic coupling in the presence of a bosonic reservoir and an Ohmic dissipation model, analyzing the evolution equation for the mean value of the oscillator coordinate. In the asymptotic case we obtain a gain-loss master equation whose transition rates are polynomials in the number of quanta. No explicit solutions other than the equilibrium one can be written, since the standard methods do not apply. The equilibrium solution is investigated and the eigenvalues of the corresponding spectral problem are numerically computed to study the effect of the nonlinearity on the evolution of the system. By means of the Wigner transformation of the GME, we extract a third-order partial derivative equation that represents the semiclassical evolution of the damped oscillator. In the classical limit this is a nonlinear Fokker-Planck equation.
The quantum Fokker-Planck equation for a Gaussian-Markovian bath is deduced by applying a method proposed by Tanimura and Kubo [J. Phys. Soc. Jpn. 58, 101 (1989)]. The results are expressed in the form of simultaneous differential equations in terms of density operators and can treat strong system-bath interactions where the correlated effects of the noise play an important role. The classical Fokker-Planck equation for a Gaussian-Markovian noise is obtained by performing the Wigner transformation, and its equilibrium state is shown to be the Maxwell-Boltzmann distribution. The method is convenient for numerical studies. Calculations for quantum-system harmonic oscillators and the double-well potential problems are demonstrated for cases of Gaussian-white noise and Gaussian-Markovian noise.