In Chapter I of this dissertation, we present a pedagogical introduction to the basic concepts of stochastic theory and review the progress made as well as the outstanding unsolved problems in the field. For the rest of this dissertation, we use a generalized quantum Langevin equation (GLE) approach to investigate various properties of quantum dissipative systems. In Chapter II, calculations for the displacement and random force correlation functions for Brownian motion are generalized to the case of an arbitrary heat bath for a damped harmonic quantum oscillator. The mean square displacement of such an oscillator is then evaluated for both Ohmic and blackbody radiation heat baths, to determine the effects of many parameters on the localization of the oscillator. In Chapter III, the formalism is extended to the Brownian motion of a charged particle in an external magnetic field as well as in a potential. The influence of the magnetic field on the memory function and random force is determined, with the blackbody radiation heat bath analyzed as a special case. For a charged harmonic oscillator, the generalized susceptibility is obtained, which enables us to derive the symmetrized position correlation functions using the fluctuation-dissipation theorem. In addition, we obtain the free energy of the system by generalizing the "remarkable formula" of Ford, Lewis, and O'Connell. Explicit calculations are performed for Ohmic and blackbody radiation heat baths. Furthermore, the effect of dissipation on the localization of the oscillator in an Ohmic heat bath at zero temperature is shown to differ qualitatively from that without the magnetic field. Finally, we formulate retarded Green's functions and symmetrized position correlation functions for the oscillator, reach some general conclusions, and make explicit calculations for the Ohmic heat bath. For the special case of Brownian motion at both zero and nonzero temperatures, we prove two general asymptotic relations between the retarded Green's functions and the displacement correlation functions, which we use to evaluate the long-time behaviors of the latter from those of the former, for both the Ohmic heat bath and a rather general class of heat baths discussed extensively in the literature.
In Chapter I of this dissertation, we present a pedagogical introduction to the basic concepts of stochastic theory and review the progress made as well as the outstanding unsolved problems in the field. For the rest of this dissertation, we use a generalized quantum Langevin equation (GLE) approach to investigate various properties of quantum dissipative systems. In Chapter II, calculations for the displacement and random force correlation functions for Brownian motion are generalized to the case of an arbitrary heat bath for a damped harmonic quantum oscillator. The mean square displacement of such an oscillator is then evaluated for both Ohmic and blackbody radiation heat baths, to determine the effects of many parameters on the localization of the oscillator. In Chapter III, the formalism is extended to the Brownian motion of a charged particle in an external magnetic field as well as in a potential. The influence of the magnetic field on the memory function and random force is determined, with the blackbody radiation heat bath analyzed as a special case. For a charged harmonic oscillator, the generalized susceptibility is obtained, which enables us to derive the symmetrized position correlation functions using the fluctuation-dissipation theorem. In addition, we obtain the free energy of the system by generalizing the "remarkable formula" of Ford, Lewis, and O'Connell. Explicit calculations are performed for Ohmic and blackbody radiation heat baths. Furthermore, the effect of dissipation on the localization of the oscillator in an Ohmic heat bath at zero temperature is shown to differ qualitatively from that without the magnetic field. Finally, we formulate retarded Green's functions and symmetrized position correlation functions for the oscillator, reach some general conclusions, and make explicit calculations for the Ohmic heat bath. For the special case of Brownian motion at both zero and nonzero temperatures, we prove two general asymptotic relations between the retarded Green's functions and the displacement correlation functions, which we use to evaluate the long-time behaviors of the latter from those of the former, for both the Ohmic heat bath and a rather general class of heat baths discussed extensively in the literature.
In a paper with the same title as the above, Manoliu and Kittel calculated the high temperature ensemble average of the nonequal time product of the displacement and random force in the classical Brownian motion problem. Here, using a generalized quantum Langevin equation (GLE), we generalize these considerations to the quantum case and to the case of an arbitrary heat bath (such as, e.g., the blackbody radiation heat bath). Also, we consider an arbitrary temperature and we generalize beyond Brownian motion to the case of a harmonically bound particle in a heat bath. In addition, we point out that correlations of the type considered are widely used in many applications in a variety of different areas of physics and we review some recent applications of the GLE.
The macroscopic description of a quantum particle with passive dissipation and moving in an arbitrary external potential is formulated in terms of the generalized Langevin equation. The coupling with the heat bath corresponds to two terms: a mean force characterized by a memory function \ensuremath{\mu}(t) and an operator-valued random force. Explicit expressions are given for the correlation and commutator of the random force. The random force is never Markovian. It is shown that \ensuremath{\mu}\ifmmode \tilde{}\else \~{}\fi{}(z), the Fourier transform of the memory function, must be a positive real function, analytic in the upper half-plane and with Re[\ensuremath{\mu}\ifmmode \tilde{}\else \~{}\fi{}(\ensuremath{\omega}+i0+)] a positive distribution on the real axis. This form is then derived for the independent-oscillator model of a heat bath. It is shown that the most general quantum Langevin equation can be realized by this simple model. A critical comparison is made with a number of other models that have appeared in the literature.
Abstract This review provides a brief and quick introduction to the quantum Langevin equation for an oscillator, while focusing on the steady-state thermodynamic aspects. A derivation of the quantum Langevin equation is carefully outlined based on the microscopic model of the heat bath as a collection of a large number of independent quantum oscillators, the so-called independent-oscillator model. This is followed by a discussion on the relevant ‘weak-coupling’ limit. In the steady state, we analyze the quantum counterpart of energy equipartition theorem which has generated a considerable amount of interest in recent literature. The free energy, entropy, specific heat, and third law of thermodynamics are discussed for one-dimensional quantum Brownian motion in a harmonic well. Following this, we explore some aspects of dissipative diamagnetism in the context of quantum Brownian oscillators, emphasizing upon the role of confining potentials and also upon the environment-induced classical-quantum crossover. We discuss situations where the system-bath coupling is via the momentum variables by focusing on a gauge-invariant model of momentum-momentum coupling in the presence of a vector potential; for this problem, we derive the quantum Langevin equation and discuss quantum thermodynamic functions. Finally, the topic of fluctuation theorems is discussed (albeit, briefly) in the context of classical and quantum cyclotron motion of a particle coupled to a heat bath.
A wide variety of dissipative and fluctuation problems involving a quantum system in a heat bath can be described by the independent-oscillator (IO) model Hamiltonian. Using Heisenberg equations of motion, this leads to a generalized quantum Langevin equation (QLE) for the quantum system involving two quantities which encapsulate the properties of the heat bath. Applications include: atomic energy shifts in a blackbody radiation heat bath; solution of the problem of runaway solutions in QED; electrical circuits (resistively shunted Josephson barrier, microscopic tunnel junction, etc.); conductivity calculations (since the QLE gives a natural separation between dissipative and fluctuation forces); dissipative quantum tunneling; noise effects in gravitational wave detectors; anomalous diffusion; strongly driven quantum systems; decoherence phenomena; analysis of Unruh radiation and entropy for a dissipative system.
The thesis comprises two major themes of quantum statistical dynamics. One is the development of quantum dissipation theory (QDT). It covers the establishment of some basic relations of quantum statistical dynamics, the construction of several nonequivalent complete second-order formulations, and the development of exact QDT. Another is related to the applications of quantum statistical dynamics to a variety of research fields. In particular, unconventional but novel theories of the electron transfer in Debye solvents, quantum transport, and quantum measurement are developed on the basis of QDT formulations. The thesis is organized as follows. In Chapter 1, we present some background knowledge in relation to the afore-mentioned two themes of this thesis. The key quantity in QDT is the reduced density operator ρ(t) ≡ trBρT(t); i.e., the partial trace of the total system and bath composite ρT(t) over the bath degrees of freedom. QDT governs the evolu-tion of reduced density operator, where the effects of bath are treated in a quantum statistical manner. In principle, the reduced density operator contains all dynam-ics information of interest. However, the conventional quantum transport theory is formulated in terms of nonequilibrium Green's function. The newly emerging field of quantum measurement in relation to quantum information and quantum computing does exploit a sort of QDT formalism. Besides the background of the relevant theoretical development, some representative experiments on molecular nanojunctions are also briefly discussed. In Chapter 2, we outline some basic (including new) relations that highlight several important issues on QDT. The content includes the background of nonequi-librium quantum statistical mechanics, the general description of the total compos-ite Hamiltonian with stochastic system-bath interaction, a novel parameterization scheme for bath correlation functions, a newly developed exact theory of driven Brownian oscillator (DBO) systems, and its closely related solvation mode trans-formation of system-bath coupling Hamiltonian in general. The exact QDT of DBO systems is also used to clarify the validity of conventional QDT formulations that involve Markovian approximation. In Chapter 3, we develop three nonequivalent but all complete second-order QDT (CS-QDT) formulations. Two of them are of the conventional prescriptions in terms of time-local dissipation and memory kernel, respectively. The third one is called the correlated driving-dissipation equations of motion (CODDE). This novel CS-QDT combines the merits of the former two for its advantages in both the application and numerical implementation aspects. Also highlighted is the importance of correlated driving-dissipation effects on the dynamics of the reduced system. In Chapter 4, we construct an exact QDT formalism via the calculus on path integrals. The new theory aims at the efficient evaluation of non-Markovian dis-sipation beyond the weak system-bath interaction regime in the presence of time-dependent external field. By adopting exponential-like expansions for bath corre-lation function, hierarchical equations of motion formalism and continued fraction Liouville-space Green's function formalism are established. The latter will soon be used together with the Dyson equation technique for an efficient evaluation of non-perturbative reduced density matrix dynamics. The interplay between system-bath interaction strength, non-Markovian property, and the required level of hierarchy is also studied with the aid of simple spin-boson systems, together with the three proposed schemes to truncate the infinite hierarchy. In Chapter 5, we develop a nonperturbative theory of electron transfer (ET) in Debye solvents. The resulting exact and analytical rate expression is constructed on the basis of the aforementioned continued fraction Liouville-space Green's func-tion formalism, together with the Dyson equation technique. Not only does it re-cover the celebrated Marcus' inversion and Kramers' turnover behaviors, the new theory also shows some distinct quantum solvation effects that can alter the ET mechanism. Moreover, the present theory predicts further for the ET reaction ther-modynamics, such as equilibrium Gibbs free-energy and entropy, some interesting solvent-dependent features that are calling for experimental verification. In Chapter 6, we discuss the constructed QDTs, in terms of their unified math-ematical structure that supports a linear dynamics space, and thus facilitates their applications to various physical problems. The involving details are exemplified with the CODDE form of QDT. As the linear space is concerned, we identify the Schrödinger versus Heisenberg picture and the forward versus backward propaga-tion of the reduced, dissipative Liouville dynamics. For applications we discuss the reduced linear response theory and the optimal control problems, in which the correlated effects of non-Markovian dissipation and field driving are shown to be important. In Chapter 7, we turn to quantum transport, i.e. electric current through molecular or mesoscopic systems under finite applied voltage. By viewing the nonequilibrium transport setup as a quantum open system, we develop a reduced-density-matrix approach to quantum transport. The resulting current is explicitly expressed in terms of the molecular reduced density matrix by tracing out the degrees of freedom of the electrodes at finite bias and temperature. We propose a conditional quantum master equation theory, which is an extension of the conven-tional (or unconditional) QDT by tracing out the well-defined bath subsets indi-vidually, instead of the entire bath degrees of freedom. Both the current and the noise spectrum can be conveniently analyzed in terms of the conditional reduced density matrix dynamics. By far, the QDT (including the conditional one) has only been exploited in a second-order form. A self-consistent Born approximation for the system-electrode coupling is further proposed to recover all existing nonlinear current-voltage behaviors including the nonequilibrium Kondo effect. Transport theory based on the exact QDT formalism will be developed in future. In Chapter 8, we study the quantum measurement of a qubit with a quantum-point-contact detector. On the basis of a unified quantum master equation (a form of QDT), we study the measurement-induced relaxation and dephasing of the qubit . Our treatment pays particular attention on the detailed-balance relation, which is a consequence of properly accounting for the energy exchange between the qubit and detector during the measurement process. We also derive a conditional quantum master equation for quantum measurement in general, and study the readout characteristics of the qubit measurement. Our theory is applicable to the quantum measurement at arbitrary voltage and temperature. A number of remarkable new features are found and highlighted in concern with their possible relevance to future experiments. In Chapter 9, we discuss the further development of QDT, aiming at an effi-cient evaluation of many-electron systems. This will be carried out by reducing the many-particle (Fermion or Boson) QDT to a single-particle one by exploring, e.g. the Wick's contraction theorem. It also results in a time-dependent density func-tional theory (TDDFT) for transport through complex large-scale (e.g. molecules) systems. Primary results of the TDDFT-QDT are reported. In Chapter 10, we summary the thesis, and comment and remark on the future work on both the theoretical and application aspects of QDT.
Quantum diffusion equations featuring explicitly time-dependent transport coefficients are derived from generalized non-Markovian Langevin equations. Generalized fluctuation-dissipation relations and analytic expressions for calculating the friction and diffusion coefficients in nuclear processes are obtained. The asymptotic behavior of the transport coefficients and correlation functions for a damped harmonic oscillator that is linearly coupled in momentum to a heat bath is studied. The coupling to a heat bath in momentum is responsible for the appearance of the diffusion coefficient in coordinate. The problem of regression of correlations in quantum dissipative systems is analyzed.