Finite-Time Dynamical Phase Transition in Nonequilibrium Relaxation

in Physical Review Letters (2022), 128(11), 110603

Thermodynamics of concentration vs flux control in chemical reaction networks

in J. Chem. Phys. (2022), 156(1), 014116

Post-thermalization via information spreading in open quantum systems

in Physical Review. E, Statistical Physics, Plasmas, Fluids, and Related Interdisciplinary Topics (2022), 106(1), 014122

Large deviations theory for noisy nonlinear electronics: CMOS inverter as a case study

in Physical Review. B, Condensed Matter and Materials Physics (2022), 106(15), 155303

Free-energy transduction in chemical reaction networks: From enzymes to metabolism

in J. Chem. Phys. (2022), 157(2), 024109

Beyond thermodynamic uncertainty relations: nonlinear response, error-dissipation trade-offs, and speed limits

in J. Phys. A: Math. Theor. (2022), 55(12), 124002

Kinetic and energetic insights into the dissipative non-equilibrium operation of an autonomous light-powered supramolecular pump

in Nature Nanotechnology (2022)

Natural and artificial autonomous molecular machines operate by constantly dissipating energy coming from an external source to maintain a non-equilibrium state. Quantitative thermodynamic ... [more ▼]

Natural and artificial autonomous molecular machines operate by constantly dissipating energy coming from an external source to maintain a non-equilibrium state. Quantitative thermodynamic characterization of these dissipative states is highly challenging as they exist only as long as energy is provided. Here we report on the detailed physicochemical characterization of the dissipative operation of a supramolecular pump. The pump transduces light energy into chemical energy by bringing self-assembly reactions to non-equilibrium steady states. The composition of the system under light irradiation was followed in real time by 1H NMR for four different irradiation intensities. The experimental composition and photon flow were then fed into a theoretical model describing the non-equilibrium dissipation and the energy storage at the steady state. We quantitatively probed the relationship between the light energy input and the deviation of the dissipative state from thermodynamic equilibrium in this artificial system. Our results provide a testing ground for newly developed theoretical models for photoactivated artificial molecular machines operating away from thermodynamic equilibrium. [less ▲]

Insights from an information thermodynamics analysis of a synthetic molecular motor

in Nature Chemistry (2022), 14(5), 530-537

Information is physical, a realization that has transformed the physics of measurement and communication. However, the flow between information, energy and mechanics in chemical systems remains largely ... [more ▼]

Information is physical, a realization that has transformed the physics of measurement and communication. However, the flow between information, energy and mechanics in chemical systems remains largely unexplored. Here we analyse a minimalist autonomous chemically driven molecular motor in terms of information thermodynamics, a framework that quantitatively relates information to other thermodynamic parameters. The treatment reveals how directional motion is generated by free energy transfer from chemical to mechanical (conformational and/or co-conformational) processes by `energy flow' and `information flow'. It provides a thermodynamic level of understanding of molecular motors that is general, complements previous analyses based on kinetics and has practical implications for machine design. In line with kinetic analysis, we find that power strokes do not affect the directionality of chemically driven machines. However, we find that power strokes can modulate motor velocity, the efficiency of free energy transfer and the number of fuel molecules consumed per cycle. This may help explain the role of such (co-)conformational changes in biomachines and illustrates the interplay between energy and information in chemical systems. [less ▲]

Nonequilibrium thermodynamics of light-induced reactions

in Journal of Chemical Physics (2021), 155

Current formulations of nonequilibrium thermodynamics of open chemical reaction networks only consider chemostats as free-energy sources sustaining nonequilibrium behaviors. Here, we extend the theory to ... [more ▼]

Current formulations of nonequilibrium thermodynamics of open chemical reaction networks only consider chemostats as free-energy sources sustaining nonequilibrium behaviors. Here, we extend the theory to include incoherent light as a source of free energy. We do so by relying on a local equilibrium assumption to derive the chemical potential of photons relative to the system they interact with. This allows us to identify the thermodynamic potential and the thermodynamic forces driving light-reacting chemical systems out-of-equilibrium. We use this framework to treat two paradigmatic photochemical mechanisms describing light-induced unimolecular reactions—namely, the adiabatic and diabatic mechanisms—and highlight the different thermodynamics they lead to. Furthermore, using a thermodynamic coarse-graining procedure, we express our findings in terms of commonly measured experimental quantities, such as quantum yields. [less ▲]

Local detailed balance across scales: From diffusions to jump processes and beyond

in Physical Review. E. (2021), 103