Nonequilibrium Work Relations and Response Theories in Ensemble Quantum Systems
Author(s)
Dodin, Amro; Willard, Adam P
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We develop a nonequilibrium response theory for macroscopic quantum systems that separates the contributions of ensemble heterogeneity and intrinsic quantum uncertainty. To accomplish this, we describe systems with a quantum P-ensemble, which goes beyond the standard density matrix description by explicitly specifying the classical heterogeneity between individual quantum systems in an ensemble. We use the P-ensemble formalism to present quantum generalizations of linear response theory and the Jarzynski nonequilibrium work relation. We derive these generalizations from a Bochkov-Kuzovlev generating functional for quantum P-ensembles, which can be further utilized to derive all orders of response theory that apply to ensemble quantum systems. We contrast these developments with their ρ-ensemble analogs, and we discuss how these P-ensemble theories provide a guide for an effective application of single molecule experiments.
Date issued
2021-11-18Department
Massachusetts Institute of Technology. Department of ChemistryJournal
The Journal of Physical Chemistry Letters
Publisher
American Chemical Society (ACS)
Citation
Dodin, Amro and Willard, Adam P. 2021. "Nonequilibrium Work Relations and Response Theories in Ensemble Quantum Systems." The Journal of Physical Chemistry Letters, 12 (45).
Version: Final published version