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arXiv:cond-mat/0309498 · Physical Review E

Quantum version of free-energy–irreversible-work relations

Wojciech De Roeck, Christian Maes

Published Feb 26, 2004• 100 citations
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Abstract

We give a quantum version of the Jarzynski relation between the distribution of work done over a certain time-interval on a system and the difference of equilibrium free energies. The main ingredient is the identification of work depending on the quantum history of the system and the proper definition of various quantum ensembles over which the averages should be made. We also discuss a number of different regimes that have been considered by other authors and which are unified in the present set-up. In all cases, quantum or classical, it is a general relation between heat and time-reversal that makes the Jarzynski relation so universally valid.

DOI
10.1103/physreve.69.026115

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We give a quantum version of the Jarzynski relation between the distribution of work done over a certain time-interval on a system and the difference of equilibrium free energies. The main ingredient is the identification of work depending on the quantum history of the system and the proper definition of various quantum ensembles over which the averages should be made. We also discuss a number of different regimes that have been considered by other authors and which are unified in the present set-up. In all cases, quantum or classical, it is a general relation between heat and time-reversal that makes the Jarzynski relation so universally valid.
The validity of the Jarzynski equation for a very simple, exactly solvable quantum system is analyzed. The implications of two different definitions of work proposed in the literature are investigated. The first one derives from measurements of the system energy at the beginning and at the end of the process under consideration making the work a classical stochastic variable with transition probabilities derived from quantum-mechanics. In the second definition an operator of work is introduced and the average in the Jarzynski equation is a quantum expectation value. For the first definition a general quantum-mechanical version of the Jarzynski equation is known to hold. For the second one the Jarzynski equation fails to yield the free energy difference at low temperature.
The universal quantum work relation connects a functional of an arbitrary observable averaged over the forward process to the free-energy difference and another functional averaged over the time-reversed process. Here, we ask the question if the system is driven out of equilibrium by a different Hamiltonian rather than the original one during the forward process and similarly during the reversed process then how accurate is the quantum work relation. We present an inequality that must be satisfied when the system is driven out by such a trial Hamiltonian. This also answers the issue of accuracy of the Jarzynski relation with a trial Hamiltonian. We have shown that the correction term can be expressed as the averages of the difference operator between the accurate and trial Hamiltonians. This leads to a generalized version of the Bogoliubov inequality for the free-energy differences.
A result of great theoretical and experimental interest, the Jarzynski equality predicts a free energy change $\mathrm{\ensuremath{\Delta}}F$ of a system at inverse temperature $\ensuremath{\beta}$ from an ensemble average of nonequilibrium exponential work, i.e., $\ensuremath{\langle}{e}^{\ensuremath{-}\ensuremath{\beta}W}\ensuremath{\rangle}={e}^{\ensuremath{-}\ensuremath{\beta}\mathrm{\ensuremath{\Delta}}F}$. The number of experimental work values needed to reach a given accuracy of $\mathrm{\ensuremath{\Delta}}F$ is determined by the variance of ${e}^{\ensuremath{-}\ensuremath{\beta}W}$, denoted $\mathrm{var}({e}^{\ensuremath{-}\ensuremath{\beta}W})$. We discover in this work that $\mathrm{var}({e}^{\ensuremath{-}\ensuremath{\beta}W})$ in both harmonic and anharmonic Hamiltonian systems can systematically diverge in nonadiabatic work protocols, even when the adiabatic protocols do not suffer from such divergence. This divergence may be regarded as a type of dynamically induced phase transition in work fluctuations. For a quantum harmonic oscillator with time-dependent trapping frequency as a working example, any nonadiabatic work protocol is found to yield a diverging $\mathrm{var}({e}^{\ensuremath{-}\ensuremath{\beta}W})$ at sufficiently low temperatures, markedly different from the classical behavior. The divergence of $\mathrm{var}({e}^{\ensuremath{-}\ensuremath{\beta}W})$ indicates the too-far-from-equilibrium nature of a nonadiabatic work protocol and makes it compulsory to apply designed control fields to suppress the quantum work fluctuations in order to test the Jarzynski equality.
We first derive the Jarzynski relation [1] between the average exponential of the thermodynamical work and the exponential of the difference between the initial and final free energy. We then comment on the information-theoretic underpinning of Jarzynski’s reasoning which helps explain why the Jarzynski relation holds identically both quantumly and classically [2]. We then present a scheme to verify the quantum non-equilibrium fluctuation relations as encapsulated by Jarzynski. We show that the characteristic function of the work distribution of a quantum system (which is basically equal to the Wick rotated average exponential of the thermodynamical work) can be extracted from Ramsey interferometry of a single probe qubit (which need not itself be pure, though it must not be fully depolarized) [3,4].We first derive the Jarzynski relation [1] between the average exponential of the thermodynamical work and the exponential of the difference between the initial and final free energy. We then comment on the information-theoretic underpinning of Jarzynski’s reasoning which helps explain why the Jarzynski relation holds identically both quantumly and classically [2]. We then present a scheme to verify the quantum non-equilibrium fluctuation relations as encapsulated by Jarzynski. We show that the characteristic function of the work distribution of a quantum system (which is basically equal to the Wick rotated average exponential of the thermodynamical work) can be extracted from Ramsey interferometry of a single probe qubit (which need not itself be pure, though it must not be fully depolarized) [3,4]. An interesting fact is that while the quantum version of the Jarzynski equality remains satisfied even in the presence of quantum correlations, the individual thermodynamical work moments in the expansion of the free energy are, in fact, sensitive to the genuine quantum correlations [5]. Whether this is a fortuitous coincidence remains to be seen, but it certainly goes towards explaining why the laws of thermodynamics happen to be so robust as to be independent of the underlying micro-physics.We intend to elucidate the subtle connection between Jarzynski’s relation and the “quantum arrow of time”. Finally we comment on the fact that our scheme for measuring the quantum work characteristic function belongs to the computational class known as DCQ1 [6], namely all computations that can be performed with only one pure qubit (and N maximally mixed ones).
A central topic in the emerging field of quantum thermodynamics is the definition of thermodynamic work in the quantum regime. One widely used solution is to define work for a closed system undergoing non-equilibrium dynamics according to the two-point energy measurement scheme. However, due to the invasive nature of measurement the two-point quantum work probability distribution cannot describe the statistics of energy change from the perspective of the system alone. We here introduce the quantum histories framework as a method to characterise the thermodynamic properties of the unmeasured , closed dynamics. Constructing continuous power operator trajectories allows us to derive an alternative quantum work distribution for closed quantum dynamics that fulfils energy conservation and is time-reversal symmetric. This opens the possibility to compare the measured work with the unmeasured work, contrasting with the classical situation where measurement does not affect the work statistics. We find that the work distribution of the unmeasured dynamics leads to deviations from the classical Jarzynski equality and can have negative values highlighting distinctly non-classical features of quantum work.
There are two related theorems which hold even in far from equilibrium, namely fluctuation theorem and Jarzynski equality. Fluctuation theorem states the existence of symmetry of fluctuation of entropy production, while the Jarzynski equality enables us to estimate the free energy change between two states by using irreversible processes. On the other hand, the relationship between these theorems was investigated by Crooks [Phys. Rev. E 60, 2721 (1999)] for the classical stochastic systems. In this paper, we derive quantum analogues of fluctuation theorem and Jarzynski equality in terms of microscopic reversibility. In other words, the quantum analog of the work by Crooks is presented. Also, for the quasiclassical Langevin system, microscopically reversible condition is confirmed.