A phase-space representation of Bloch–Redfield theory is used to describe the dynamical evolution of quantum dissipative systems. The resulting Liouville operator equations are capable of incorporating both the master equation in eigenstate space and the stochastic equation in classical phase space, and thus provide a useful framework for mixing classical, semiclassical, and quantum dynamics for simulating complicated dissipative systems. In addition, the proper limit of quantum dissipation, the approximate nature of the second-order cumulant truncation, the detailed balance of quantum correlation functions, and the reduction of dissipation by a transformation of the bath Hamiltonian are investigated within the framework of phase-space Bloch–Redfield theory.
A phase-space representation of Bloch–Redfield theory is used to describe the dynamical evolution of quantum dissipative systems. The resulting Liouville operator equations are capable of incorporating both the master equation in eigenstate space and the stochastic equation in classical phase space, and thus provide a useful framework for mixing classical, semiclassical, and quantum dynamics for simulating complicated dissipative systems. In addition, the proper limit of quantum dissipation, the approximate nature of the second-order cumulant truncation, the detailed balance of quantum correlation functions, and the reduction of dissipation by a transformation of the bath Hamiltonian are investigated within the framework of phase-space Bloch–Redfield theory.
Six major theories of quantum dissipative dynamics are compared: Redfield theory, the Gaussian phase space ansatz of Yan and Mukamel, the master equations of Agarwal, Caldeira-Leggett/Oppenheim-Romero-Rochin, and Louisell/Lax, and the semigroup theory of Lindblad. The time evolving density operator from each theory is transformed into a Wigner phase space distribution, and classical-quantum correspondence is investigated via comparison with the phase space distribution of the classical Fokker-Planck (FP) equation. Although the comparison is for the specific case of Markovian dynamics of the damped harmonic oscillator with no pure dephasing, certain inferences can be drawn about general systems. The following are our major conclusions: (1) The harmonic oscillator master equation derived from Redfield theory, in the limit of a classical bath, is identical to the Agarwal master equation. (2) Following Agarwal, the Agarwal master equation can be transformed to phase space, and differs from the classical FP equation only by a zero point energy in the diffusion coefficient. This analytic solution supports Gaussian solutions with the following properties: the differential equations for the first moments in p and q and all but one of the second moments (q2 and pq but not p2) are identical to the classical equations. Moreover, the distribution evolves to the thermal state of the bare quantum system at long times. (3) The Gaussian phase space ansatz of Yan and Mukamel (YM), applied to single surface oscillator dynamics, reduces to the analytical Gaussian solutions of the Agarwal phase space master equation. It follows that the YM ansatz is also a solution to the Redfield master equation. (4) The Agarwal/Redfield master equation has a structure identical to that of the master equation of Caldeira-Leggett/Oppenheim-Romero-Rochin, but the two are equivalent only in the high temperature limit. (5) The Louisell/Lax HO master equation differs from the Agarwal/Redfield form by making a rotating wave approximation (RWA), i.e., keeping terms of the form ââ†,â†â and neglecting terms of the form â†â†,ââ. When transformed into phase space, the neglect of these terms eliminates the modulation in time of the energy dissipation, modulation which is present in the classical solution. This neglect leads to a position-dependent frictional force which violates the principle of translational invariance. (6) The Agarwal/Redfield (AR) equations of motion are shown to violate the semigroup form of Lindblad required for complete positivity. Considering the triad of properties: complete positivity, translational invariance and asymptotic approach to thermal equilibrium, AR sacrifices the first while Lindblad’s form must sacrifice either the second or the third. This implies that for certain initial states Redfield theory can violate simple positivity; however, for a wide range of initial Gaussians, the solution of the AR equations does maintain simple positivity, and thus for these states appears to be distinctly more physical than the solution of the semigroup equations.
Classical Brownian motion has well been investigated since the pioneering work of Einstein, which inspired mathematicians to lay the theoretical foundation of stochastic processes. A stochastic formulation for quantum dynamics of dissipative systems described by the system-plus-bath model has been developed and found many applications in chemical dynamics, spectroscopy, quantum transport, and other fields. This article provides a tutorial review of the stochastic formulation for quantum dissipative dynamics. The key idea is to decouple the interaction between the system and the bath by virtue of the Hubbard-Stratonovich transformation or Itô calculus so that the system and the bath are not directly entangled during evolution, rather they are correlated due to the complex white noises introduced. The influence of the bath on the system is thereby defined by an induced stochastic field, which leads to the stochastic Liouville equation for the system. The exact reduced density matrix can be calculated as the stochastic average in the presence of bath-induced fields. In general, the plain implementation of the stochastic formulation is only useful for short-time dynamics, but not efficient for long-time dynamics as the statistical errors go very fast. For linear and other specific systems, the stochastic Liouville equation is a good starting point to derive the master equation. For general systems with decomposable bath-induced processes, the hierarchical approach in the form of a set of deterministic equations of motion is derived based on the stochastic formulation and provides an effective means for simulating the dissipative dynamics. A combination of the stochastic simulation and the hierarchical approach is suggested to solve the zero-temperature dynamics of the spin-boson model. This scheme correctly describes the coherent-incoherent transition (Toulouse limit) at moderate dissipation and predicts a rate dynamics in the overdamped regime. Challenging problems such as the dynamical description of quantum phase transition (local- ization) and the numerical stability of the trace-conserving, nonlinear stochastic Liouville equation are outlined.
A quantum-classical approximation, capable of describing the evolution of open quantum systems well beyond the applicability limits of Redfield theory is suggested. The theory is based on the short lifetime of the quantum correlations between the quantum and the classical subsystem, caused by energy dispersion (per degree of freedom) of the canonical bath. The resulting quantum-classical approximation has the form of two auxiliary differential equations and fully accounts both for the arbitrary long memory of the heat reservoir and detailed balance. These equations allow direct solution in the time domain without constructing/diagonalizing Liouville space operators, and, in combination with molecular dynamics techniques to simulate bath dynamics, may be applied to quantum subsystems with a fairly large number of levels. A simple example of a two-level system, coupled to a single correlation time canonical bath, was considered to demonstrate different regimes of approaching the canonical equilibrium state.
A semiclassical approximation for an evolving density operator, driven by a “closed” hamiltonian operator and “open ” markovian Lindblad operators, is obtained. The theory is based on the chord function, i.e. the Fourier transform of the Wigner function. It reduces to an exact solution of the Lindblad master equation if the hamiltonian operator is a quadratic function and the Lindblad operators are linear functions of positions and momenta. Initially, the semiclassical formulae for the case of hermitian Lindblad operators are reinterpreted in terms of a (real) double phase space, generated by an appropriate classical double Hamiltonian. An extra “open ” term is added to the double Hamiltonian by the non-hermitian part of the Lindblad operators in the general case of dissipative markovian evolution. The particular case of generic hamiltonian operators, but linear dissipative Lindblad operators, is studied in more detail. A Liouville-type equivariance still holds for the corresponding classical evolution in double phase, but the centre subspace, which supports the Wigner function, is compressed, along with expansion of its conjugate subspace, which supports the chord function. Decoherence narrows the relevant region of double phase space to the neighborhood of a caustic for both the Wigner function and the chord function. This difficulty is avoided by a propagator in a mixed representation, so that a further “small-chord” approximation leads to a simple generalization of the quadratic theory for evolving Wigner functions.
We systematically investigate master equations involving double-bracket dissipators in the classical limit. Dissipators defined by double commutators arise naturally in dephasing dynamics, while those defined by double anticommutators are typically associated with noisy Hamiltonians. The classical limit of such master equations is derived by reformulating the dissipative open dynamics in phase space using the Wigner-Weyl transform and Moyal bracket formalism, and by identifying the leading-order terms in a systematic ℏ-expansion. We first analyze a double-commutator master equation associated with energy diffusion, and then turn to master equations containing a double anticommutator with the system Hamiltonian, recently derived in the context of noisy non-Hermitian systems. For both classes of double-bracket equations, we establish a gradient-flow representation of the dynamics within both the quantum and semiclassical formalisms. We further study the semiclassical evolution generated by double-bracket master equations for the harmonic (integrable) and driven anharmonic (chaotic) oscillators, considering both classical and quantum initial states. The dynamics are characterized through several observables, including mean position, momentum, and energy. The quantumness of the time-evolved state is assessed via the Wigner logarithmic negativity, and the interplay between double-bracket dissipation and chaotic dynamics is examined in detail. Finally, we extend our analysis to generalized master equations involving higher-order nested brackets, which arise naturally as a time-continuous formulation of spectral filtering techniques widely used in the numerical simulation of quantum systems.
A quantum dissipation theory is constructed with the system–bath interaction being treated rigorously at the second-order cumulant level for both reduced dynamics and initial canonical boundary condition. The theory is valid for arbitrary bath correlation functions and time-dependent external driving fields, and satisfies correlated detailed-balance relation at any temperatures. The general formulation assumes a particularly simple form in driven Brownian oscillator systems in which the correlated driving-dissipation effects can be accounted for exactly in terms of local-field correction. Remarks on a class of widely used phenomenological quantum master equations that neglects the bath dispersion-induced dissipation are also made in contact with the present theory.