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arXiv:2504.12202 · Physical Review A

Correlated dynamics as a resource in molecular switches

Daniel Siciliano, Rudi B. P. Pietsch, Giovanni Spaventa, Susana F. Huelga, Martin Bodo Plenio

Published Sep 5, 2025• 2 citations
arXivHTMLPDF

Abstract

Photoisomerization, a photochemical process underlying many biological mechanisms, has been modeled recently within the quantum resource theory of thermodynamics. This approach has emerged as a promising tool for studying fundamental limitations to nanoscale processes independently of the microscopic details governing their dynamics. On the other hand, correlations between physical systems have been shown to play a crucial role in quantum thermodynamics by lowering the work cost of certain operations. Here we explore quantitatively how correlations between multiple photoswitches can enhance the efficiency of photoisomerization beyond that attainable for single molecules. Furthermore, our analysis provides insights into the interplay between quantum and classical correlations in these transformations.

DOI
10.1103/khj7-3clh

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Photoisomerization, a photochemical process underlying many biological mechanisms, has been modeled recently within the quantum resource theory of thermodynamics. This approach has emerged as a promising tool for studying fundamental limitations to nanoscale processes independently of the microscopic details governing their dynamics. On the other hand, correlations between physical systems have been shown to play a crucial role in quantum thermodynamics by lowering the work cost of certain operations. Here we explore quantitatively how correlations between multiple photoswitches can enhance the efficiency of photoisomerization beyond that attainable for single molecules. Furthermore, our analysis provides insights into the interplay between quantum and classical correlations in these transformations.
The resource theory of quantum thermodynamics has emerged as a powerful tool for exploring the out-of-equilibrium dynamics of microscopic and highly correlated systems. Recently, it has been employed in photoisomerization, a mechanism facilitating vision through the isomerism of the photoreceptor protein rhodopsin, to elucidate the fundamental limits of efficiency inherent in this physical process. Limited attention has been given to the impact of energetic quantum coherences in this process, as these coherences do not influence the energy-level populations within an individual molecule subjected to thermal operations. However, a specific type of energetic quantum coherences can impact the energy-level populations in the scenario involving two or more molecules. In this study, we examine the case of two molecules undergoing photoisomerization to show that energetic quantum coherence can function as a resource that amplifies the efficiency of photoisomerization. These insights offer evidence for the role of energetic quantum coherence as a key resource in the realm of quantum thermodynamics at mesoscopic scales. Published by the American Physical Society 2024
Quantum resource theory formulations of thermodynamics offer a versatile tool for the study of fundamental limitations to the efficiency of physical processes, independently of the microscopic details governing their dynamics. Despite the ubiquitous presence of non-Markovian dynamics in open quantum systems at the nanoscale, rigorous proofs of their beneficial effects on the efficiency of quantum dynamical processes at the bio-molecular level have not been reported yet. Here we combine the resource theory of athermality with concepts from the theory of divisibility classes for quantum channels, to prove that memory effects can increase the efficiency of photoisomerization to levels that are not achievable under a purely thermal Markovian (i.e. memoryless) evolution. This provides rigorous evidence that memory effects can provide a resource in biological quantum dynamics, and, more generally, quantum thermodynamics at the nanoscale.
Quantum resource theory formulations of thermodynamics offer a versatile tool for the study of fundamental limitations to the efficiency of physical processes, independently of the microscopic details governing their dynamics. Despite the ubiquitous presence of non-Markovian dynamics in open quantum systems at the nanoscale, rigorous proofs of their beneficial effects on the efficiency of quantum dynamical processes at the molecular level have not been reported yet. Here we combine the quantum resource theory of athermality with concepts from the theory of divisibility classes of quantum channels to prove that memory effects can increase the efficiency of photoisomerization to levels that are not achievable under a purely thermal Markovian (i.e., memoryless) evolution. This provides rigorous evidence that memory effects can provide a resource in quantum thermodynamics at the nanoscale.
Resource-theoretic approaches to thermodynamics provide powerful, model-independent bounds on the efficiency of physical processes, because they do not rely on microscopic details of the environment. Whether such bounds can be approached by realistic dynamics generated by explicit system-environment interactions remains an open question. Photoisomerization, a fundamental molecular photoreaction, offers a concrete setting to examine this issue. We introduce a tunable microscopic model of a molecular photoswitch coupled to a structured vibrational environment, which interpolates continuously between Markovian and non-Markovian regimes. Resource-theoretic analysis predicts in particular that Markovian Thermal Operations achieve strictly lower yields than general Thermal Operations. We show that environmental memory lifts dynamical restrictions associated with Markovian thermal evolutions, thereby enlarging the set of transformations accessible to the microscopic dynamics. Approaching the thermal operation bound, however, depends on the microscopic coupling structure that generates this memory and directs the resulting dynamics towards the target transformation.
Quantum resource theory formulations of thermodynamics offer a versatile tool for the study of fundamental limitations to the efficiency of physical processes, independently of the microscopic details governing their dynamics. Despite the ubiquitous presence of non-Markovian dynamics in open quantum systems at the nanoscale, rigorous proofs of their beneficial effects on the efficiency of quantum dynamical processes at the bio-molecular level have not been reported yet. Here we combine the resource theory of athermality with concepts from the theory of divisibility classes for quantum channels, to prove that memory effects can increase the efficiency of photoisomerization to levels that are not achievable under a purely Markovian (i.e. memoryless) evolution. This provides rigorous evidence that memory effects can be a useful resource in biological quantum dynamics, and, more generally, quantum thermodynamics at the nanoscale.
Thermodynamical systems at the nanoscale, such as single molecules interacting with highly structured vibrational environments, typically undergo nonequilibrium physical processes that lack precise microscopic descriptions. Photoisomerization is such an example, which has emerged as a platform on which to study single-molecule ultrafast photochemical processes from a quantum resource theoretic perspective. However, the upper bounds on its efficiency have only been obtained under significant simplifications that make the mathematics of the resource-theoretical treatment manageable. Here we generalize previous models for the photoisomers, while retaining the full vibrational structure, and still obtain analytical bounds on the efficiency of photoisomerization. We quantify the impact of such a vibrational structure on the optimal photoisomerization quantum yield both when the vibrational coordinate has no dynamics of its own and when we take into account the vibrational dynamics. This work serves as an example of how to bridge the gap between the abstract language of quantum resource theories and the open system formulation of nanoscale processes.