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Physical review. B./Physical review. B

Strong-coupling quantum thermodynamics of quantum Brownian motion based on the exact solution of its reduced density matrix

Chuan-Zhe Yao, Weimin Zhang

Published Aug 6, 2024• 2 citations
Publisher

Abstract

The strong system-reservoir coupling prevents the thermal equilibrium state of systems from being expressed as a Gibbs state with bare system Hamiltonian. Correspondingly, many thermodynamic quantities must be redefined. In particular, for the heat capacity of strongly coupled quantum Brownian motion, there has been controversy regarding inconsistencies in different definitions and the anomalous negative heat capacity. Here, the authors rigorously solve the reduced density matrix of quantum Brownian motion and obtain the renormalized Hamiltonian and reduced partition function. This resolves the controversy about the heat capacity under strong coupling.

DOI
10.1103/physrevb.110.085114

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The strong system-reservoir coupling prevents the thermal equilibrium state of systems from being expressed as a Gibbs state with bare system Hamiltonian. Correspondingly, many thermodynamic quantities must be redefined. In particular, for the heat capacity of strongly coupled quantum Brownian motion, there has been controversy regarding inconsistencies in different definitions and the anomalous negative heat capacity. Here, the authors rigorously solve the reduced density matrix of quantum Brownian motion and obtain the renormalized Hamiltonian and reduced partition function. This resolves the controversy about the heat capacity under strong coupling.
We derive the quantum thermodynamics of quantum Brownian motion from the exact solution of its reduced density matrix. We start from the total equilibrium thermal state between the Brownian particle and its reservoir, and solve analytically and exactly the reduced density matrix of the system by taking the partial trace over all the reservoir states. We find that the reduced Hamiltonian and the reduced partition function of the Brownian motion must be renormalized significantly, as shown in the general nonperturbative renormalization theory of quantum thermodynamics for open quantum systems we developed recently [Phys. Rev. Res. 4, 023141 (2022)]. The reduced Hamiltonian contains not only a frequency shift but also a squeezing pairing interaction, where a momentum-dependent potential is generated naturally from the strong coupling between the Brownian particle and the reservoir, after traced over all the reservoir states. The resulting exact reduced density matrix of the Brownian motion is given by a squeezing thermal state. Moreover, beyond the weak coupling limit, in order to obtain correctly the reduced partition function of the Brownian motion, one must take into account the non-negligible changes of the reservoir state induced by the system-reservoir coupling. Using the exact solutions of the reduced density matrix, the reduced Hamiltonian as well as the reduced partition function of the Brownian motion, we show that the controversial results obtained from the different definitions of internal energy and the issue of the negative heat capacity in the previous studies of strong-coupling quantum thermodynamics are resolved.
By solving the exact master equation of open quantum systems, we formulate the quantum thermodynamics from weak to strong couplings. The open quantum systems exchange matters, energies, and information with their reservoirs through quantum particle tunnelings that are described by the generalized Fano-Anderson Hamiltonians. We find that the exact solution of the reduced density matrix of these systems approaches a Gibbs-type state in the steady-state limit for the systems in arbitrary initial states as well as for both the weak and strong system-reservoir coupling strengths. When the couplings become strong, thermodynamic quantities of the system must be renormalized. The renormalization effects are obtained nonperturbatively after exactly tracing over all reservoir states through the coherent state path integrals. The renormalized system Hamiltonian is characterized by the renormalized system energy levels and interactions, corresponding to the quantum work done by the system. The renormalized temperature is introduced to characterize the entropy production counting the heat transfer between the system and the reservoir. We further find that only with the renormalized system Hamiltonian and other renormalized thermodynamic quantities can the exact steady state of the system be expressed as the standard Gibbs state. Consequently, the corresponding exact steady-state particle occupations in the renormalized system energy levels obey the Bose-Einstein and the Fermi-Dirac distributions for bosonic and fermionic systems, respectively. In the very weak system-reservoir coupling limit, the renormalized system Hamiltonian and the renormalized temperature are reduced to the original bare Hamiltonian of the system and the initial temperature of the reservoir. Thus, the conventional statistical mechanics and thermodynamics are thereby rigorously deduced from quantum dynamical evolution. In the last, this nonperturbative renormalization method is also extended to general interacting open quantum systems.
We develop the strong coupling quantum thermodynamics based on the solution of the exact master equation. We find that both the Hamiltonian and the temperature must be renormalized due to the system-reservoir couplings. With the renormalized Hamiltonian and temperature, the exact steady state of open quantum systems can be expressed as a standard Gibbs state. The exact steady-state particle distributions obey the Bose-Einstein distribution or the Fermi-Dirac distribution only for the renormalized energy and temperature. In this formulation, heat and work are quantum mechanically defined, from which we compute the specific heat and examine the consistency of the theory. Consequently, thermodynamic laws and statistical mechanics emerge naturally and rigorously from quantum evolution of open systems.
Quantum systems strongly coupled to many-body systems equilibrate to the reduced state of a global thermal state, deviating from the local thermal state of the system as it occurs in the weak-coupling limit. Taking this insight as a starting point, we study the thermodynamics of systems strongly coupled to thermal baths. First, we provide strong-coupling corrections to the second law applicable to general systems in three of its different readings: As a statement of maximal extractable work, on heat dissipation, and bound to the Carnot efficiency. These corrections become relevant for small quantum systems and vanish in first order in the interaction strength. We then move to the question of power of heat engines, obtaining a bound on the power enhancement due to strong coupling. Our results are exemplified on the paradigmatic non-Markovian quantum Brownian motion.
Strong coupling generally drives a subsystem away from the Gibbs state of its bare Hamiltonian at the bath temperature. We formulate a temperature--Hamiltonian ambiguity: the reduced equilibrium state fixes the dimensionless Gibbs generator, but does not by itself uniquely determine the local Hamiltonian and temperature entering a Gibbs representation. We propose an operational resolution in which the local Hamiltonian is identified from physical information independent of the stationary Gibbs parametrization. Whenever the exact reduced state is compatible with the Gibbs family generated by that independently identified Hamiltonian, it then determines a unique local temperature. An exactly solvable two-level-system--oscillator model makes the ambiguity explicit through state-equivalent descriptions based on temperature renormalization relative to a specified local Hamiltonian and Hamiltonian-of-mean-force level renormalization at the bath temperature. An exact bosonic model provides the complementary case in which retarded dynamics independently fixes a renormalized local excitation scale and thereby specifies the local Hamiltonian before the stationary populations determine the temperature. These results distinguish state representation from thermodynamic assignment and provide an operational framework for local thermodynamics beyond weak coupling.
In a series of papers, we intend to take the perspective of open quantum systems and examine from their nonequilibrium dynamics the conditions when the physical quantities, their relations, and the laws of thermodynamics become well defined and viable for quantum many-body systems. We first describe how an open-system nonequilibrium dynamics (ONEq) approach is different from the closed combined system + environment in a global thermal state (CGTs) setup. Only after the open system equilibrates will it be amenable to conventional thermodynamics descriptions, thus quantum thermodynamics (QTD) comes at the end rather than assumed in the beginning. The linkage between the two comes from the reduced density matrix of ONEq in that stage having the same form as that of the system in the CGTs. We see the open-system approach having the advantage of dealing with nonequilibrium processes as many experiments in the near future will call for. Because it spells out the conditions of QTD's existence, it can also aid us in addressing the basic issues in quantum thermodynamics from first principles in a systematic way. We then study one broad class of open quantum systems where the full nonequilibrium dynamics can be solved exactly, that of the quantum Brownian motion of N strongly coupled harmonic oscillators, interacting strongly with a scalar-field environment. In this paper, we focus on the internal energy, heat capacity, and the third law. We show for this class of physical models, amongst other findings, the extensive property of the internal energy, the positivity of the heat capacity, and the validity of the third law from the perspective of the behavior of the heat capacity toward zero temperature. These conclusions obtained from exact solutions and quantitative analysis clearly disprove claims of negative specific heat in such systems and dispel allegations that in such systems the validity of the third law of thermodynamics relies on quantum entanglement. They are conceptually and factually unrelated issues. Entropy and entanglement will be the main theme of our second paper on this subject matter.