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arXiv:2408.13417 · Physical Review Letters

Operational Work Fluctuation Theorem for Open Quantum Systems

Konstantin Beyer, Walter T. Strunz

Published Apr 9, 2025• 2 citations
arXivHTMLPDF

Abstract

The classical Jarzynski equality establishes an exact relation between the stochastic work performed on a system driven out of thermal equilibrium and the free energy difference in a corresponding quasistatic process. This fluctuation theorem bears experimental relevance, as it enables the determination of the free energy difference through the measurement of externally applied work in a nonequilibrium process. In the quantum case, the Jarzynski equality only holds if the measurement procedure of the stochastic work is drastically changed: it is replaced by a so-called two-point measurement scheme that requires the knowledge of the initial and final Hamiltonian and therefore lacks the predictive power for the free energy difference that the classical Jarzynski equation is known for. Here, we propose a quantum fluctuation theorem that is valid for externally measurable quantum work determined during the driving protocol. In contrast to the two-point measurement case, the theorem also applies to open quantum systems and the scenario can be realized without knowing the system Hamiltonian. Our fluctuation theorem comes in the form of an inequality and therefore only yields bounds to the true free energy difference. The inequality is saturated in the quasiclassical case of vanishing energy coherences at the beginning and at the end of the protocol. Thus, there is a clear quantum disadvantage.

DOI
10.1103/physrevlett.134.140403

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The classical Jarzynski equality establishes an exact relation between the stochastic work performed on a system driven out of thermal equilibrium and the free energy difference in a corresponding quasistatic process. This fluctuation theorem bears experimental relevance, as it enables the determination of the free energy difference through the measurement of externally applied work in a nonequilibrium process. In the quantum case, the Jarzynski equality only holds if the measurement procedure of the stochastic work is drastically changed: it is replaced by a so-called two-point measurement scheme that requires the knowledge of the initial and final Hamiltonian and therefore lacks the predictive power for the free energy difference that the classical Jarzynski equation is known for. Here, we propose a quantum fluctuation theorem that is valid for externally measurable quantum work determined during the driving protocol. In contrast to the two-point measurement case, the theorem also applies to open quantum systems and the scenario can be realized without knowing the system Hamiltonian. Our fluctuation theorem comes in the form of an inequality and therefore only yields bounds to the true free energy difference. The inequality is saturated in the quasiclassical case of vanishing energy coherences at the beginning and at the end of the protocol. Thus, there is a clear quantum disadvantage.
In this Letter we propose a framework to define work as a quantum observable on a control device which is driving a system. Motivated by the conceptual difference between well known quantum versions of the Jarzynski equality (JE), where the initial and final system Hamiltonian have to be known in advance, and their classical counterparts where such knowledge is not needed, we construct a scheme where a work increment is given by an expectation value of a quantum observable on an external system. We further show that such a definition of work satisfies a fluctuation theorem which allows the free energy difference to be estimated operationally without knowledge about the Hamiltonian of the system at the end of the driving protocol. However, knowledge about the basis of the initial Hamiltonian is in general still needed. Providing two examples we describe how bounds on free energy differences could approximately be determined in experiments.
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.
Abstract Work is a process-based quantity, and its measurement typically requires interaction with a measuring device multiple times. While classical systems allow for non-invasive and accurate measurements, quantum systems present unique challenges due to the influence of the measuring device on the final value of work. As recent studies have shown, among these challenges is the impossibility of formulating a universal definition of work that respects energy conservation for coherent quantum systems and is compatible with the Jarzynski equality—a fluctuation relation linking the equilibrium free energy difference to the non-equilibrium work. Here, we overcome this challenge by introducing a genuinely quantum, positive correction to the Jarzynski equality stemming from imposing energy conservation. When sufficiently large, this correction forces quantum work to violate the second law more often. Moreover, we construct modified two-point measurement (TPM) schemes for work, along with circuit implementations for them. These measurement schemes correctly certify energy conservation and remain consistent with our quantum-corrected fluctuation relation.
Work in the paradigm of the quantum fluctuation theorems of Crooks and Jarzynski is determined by projective measurements of energy at the beginning and end of the force protocol. In analogy to classical systems, we consider an alternative definition of work given by the integral of the supplied power determined by integrating up the results of repeated measurements of the instantaneous power during the force protocol. We observe that such a definition of work, in spite of taking account of the process dependence, has different possible values and statistics from the work determined by the conventional two energy measurement approach (TEMA). In the limit of many projective measurements of power, the system’s dynamics is frozen in the power measurement basis due to the quantum Zeno effect leading to statistics only trivially dependent on the force protocol. In general the Jarzynski relation is not satisfied except for the case when the instantaneous power operator commutes with the total Hamiltonian at all times. We also consider properties of the joint statistics of power-based definition of work and TEMA work in protocols where both values are determined. This allows us to quantify their correlations. Relaxing the projective measurement condition, weak continuous measurements of power are considered within the stochastic master equation formalism. Even in this scenario the power-based work statistics is in general not able to reproduce qualitative features of the TEMA work statistics.
In this Letter we investigate the concept of quantum work and its measurability from the viewpoint of quantum measurement theory. Very often, quantum work and fluctuation theorems are discussed in the framework of projective two-point measurement (TPM) schemes. According to a well-known no-go theorem, there is no work observable which satisfies both (i) an average work condition and (ii) the TPM statistics for diagonal input states. Such projective measurements represent a restrictive class among all possible measurements. It is desirable, both from a theoretical and experimental point of view, to extend the scheme to the general case including suitably designed unsharp measurements. This shifts the focus to the question of what information about work and its fluctuations one is able to extract from such generalized measurements. We show that the no-go theorem no longer holds if the observables in a TPM scheme are jointly measurable for any intermediate unitary evolution. We explicitly construct a model with unsharp energy measurements and derive bounds for the visibility that ensure joint measurability. In such an unsharp scenario a single work measurement apparatus can be constructed that allows us to determine the correct average work and to obtain free energy differences with the help of a Jarzynski equality.
Based on the observation that the thermodynamic equilibrium free energy of an open quantum system in contact with a thermal environment is the difference between the free energy of the total system and that of the bare environment, the validity of the Crooks theorem and of the Jarzynski equality is extended to open quantum systems. No restrictions on the nature of the environment or on the strength of the coupling between system and environment need to be imposed. This free energy entering the Crooks theorem and the Jarzynski equality is closely related to the Hamiltonian of mean force that generalizes the classical statistical mechanical concept of the potential of mean force.