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Gradient and GENERIC Systems in the Space of Fluxes, Applied to Reacting Particle Systems
In a previous work we devised a framework to derive generalised gradient systems for an evolution equation from the large deviations of an underlying microscopic system, in the spirit of the Onsager–Machlup relations. Of particular interest is the case where the microscopic system consists of random particles, and the macroscopic quantity is the empirical measure or concentration. In this work we take the particle flux as the macroscopic quantity, which is related to the concentration via a continuity equation. By a similar argument the large deviations can induce a generalised gradient or GENERIC system in the space of fluxes. In a general setting we study how flux gradient or GENERIC systems are related to gradient systems of concentrations. This shows that many gradient or GENERIC systems arise from an underlying gradient or GENERIC system where fluxes rather than densities are being driven by (free) energies. The arguments are explained by the example of reacting particle systems, which is later expanded to include spatial diffusion as well.
Large deviations of reaction fluxes
We study a system of interacting particles that randomly react to form new particles. The reaction flux is the rescaled number of reactions that take place in a time interval. We prove a dynamic large-deviation principle for the reaction fluxes under general assumptions that include mass-action kinetics. This result immediately implies the dynamic large deviations for the empirical concentration.
Dynamical large deviations of countable reaction networks under a weak reversibility condition
A dynamic large deviations principle for a countable reaction network including coagulation-fragmentation models is proved. The rate function is represented as the infimal cost of the reaction fluxes and a minimiser for this variational problem is shown to exist. A weak reversibility condition is used to control the boundary behaviour and to guarantee a representation for the optimal fluxes via a Lagrange multiplier that can be used to construct the changes of measure used in standard tilting arguments. Reflecting the pure jump nature of the approximating processes, their paths are treated as elements of a BV function space.