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Fundamental limitations on photoisomerization from thermodynamic resource theories

Yunger Halpern, Nicole and Limmer, David T. (2020) Fundamental limitations on photoisomerization from thermodynamic resource theories. Physical Review A, 101 (4). Art. No. 042116. ISSN 2469-9926. doi:10.1103/PhysRevA.101.042116. https://resolver.caltech.edu/CaltechAUTHORS:20190207-150038978

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Abstract

Small, out-of-equilibrium, and quantum systems defy simple thermodynamic expressions. Such systems are exemplified by molecular switches, which exchange heat with a bath. These molecules can photoisomerize, or change conformation, or switch, on absorbing light. The photoisomerization probability depends on kinetic details that couple the molecule's energetics to its dissipation. Therefore, a simple, general, thermodynamic-style bound on the photoisomerization probability seems out of reach. We derive such a bound using a resource theory. The resource-theory framework is a set of mathematical tools, developed in quantum information theory, used to generalize thermodynamics to small and quantum settings. From this toolkit has been derived a generalization of the second law, the thermomajorization preorder. We use thermomajorization to upper-bound the photoisomerization probability. Then, we compare the bound with an equilibrium prediction and with a Lindbladian model. We identify a realistic parameter regime in which the Lindbladian evolution saturates the thermomajorization bound. We also quantify the energy coherence in the electronic degree of freedom, and we argue that this coherence cannot promote photoisomerization. This work illustrates how quantum-information-theoretic thermodynamics can elucidate complex quantum processes in nature, experiments, and synthetics.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1103/PhysRevA.101.042116DOIArticle
https://arxiv.org/abs/1811.06551arXivDiscussion Paper
ORCID:
AuthorORCID
Yunger Halpern, Nicole0000-0001-8670-6212
Limmer, David T.0000-0002-2766-0688
Additional Information:© 2020 American Physical Society. Received 9 December 2019; revised manuscript received 9 March 2020; accepted 13 March 2020; published 17 April 2020. N.Y.H. thanks Bassam Helou, David Jennings, Christopher Perry, and Mischa Woods for helpful conversations. N.Y.H. is grateful for funding from the Institute for Quantum Information and Matter, an NSF Physics Frontiers Center (NSF Grant No. PHY-1125565) with support from the Gordon and Betty Moore Foundation (GBMF-2644), for a Barbara Groce Graduate Fellowship, for a KITP Graduate Fellowship (the KITP receives support from the NSF under Grant No. NSF PHY-1125915), and for an NSF grant for the Institute for Theoretical Atomic, Molecular, and Optical Physics at Harvard University and the Smithsonian Astrophysical Observatory. D.T.L. was initially supported by the UC Berkeley College of Chemistry and by the Kavli Energy NanoSciences Institute. The later stage of this work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, CPIMS Program Early Career Research Program under Award No. DE-FOA-0002019.
Group:Institute for Quantum Information and Matter
Funders:
Funding AgencyGrant Number
NSFPHY-1125565
Gordon and Betty Moore FoundationGBMF-2644
Barbara Groce Graduate Fellowship, CaltechUNSPECIFIED
Kavli Institute for Theoretical PhysicsUNSPECIFIED
NSFPHY-1125915
Harvard UniversityUNSPECIFIED
Smithsonian Astrophysical ObservatoryUNSPECIFIED
University of California, BerkeleyUNSPECIFIED
Kavli Energy NanoSciences InstituteUNSPECIFIED
Department of Energy (DOE)DE-FOA-0002019
Issue or Number:4
DOI:10.1103/PhysRevA.101.042116
Record Number:CaltechAUTHORS:20190207-150038978
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20190207-150038978
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:92769
Collection:CaltechAUTHORS
Deposited By: Bonnie Leung
Deposited On:15 Feb 2019 21:01
Last Modified:16 Nov 2021 03:53

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