Nonequilibrium Work Relations and Response Theories in Ensemble Quantum Systems
Name
acs.jpclett.1c01315.pdf
Description
Published version
Size
769.37 KB
Format
Adobe PDF
Checksum (MD5)
8bedbe35a4ac09e315db41ce07285468
Author(s)
Dodin, Amro
Willard, Adam P
Date Issued
November 18, 2021
Journal
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
Abstract
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.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
Terms of Use
Creative Commons Attribution-NonCommercial-NoDerivs License
Persistent DSpace Link
DOI of Published Version
https://doi.org/10.1021/acs.jpclett.1c01315
