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We present a time dependent variational method to learn the mechanisms of equilibrium reactive processes and efficiently evaluate their rates within a transition path ensemble. This approach builds off variational path sampling methodology…

Chemical Physics · Physics 2023-07-10 Aditya N. Singh , David T. Limmer

Understanding chemical mechanisms requires estimating dynamical statistics such as expected hitting times, reaction rates, and committors. Here, we present a general framework for calculating these dynamical quantities by approximating…

Data Analysis, Statistics and Probability · Physics 2019-07-24 Erik H. Thiede , Dimitrios Giannakis , Aaron R. Dinner , Jonathan Weare

Stochastic models of chemical reaction networks are an important tool to describe and analyze noise effects in cell biology. When chemical species and reaction rates in a reaction system have different orders of magnitude, the associated…

Probability · Mathematics 2020-09-15 German Enciso , Jinsu Kim

A combination of a steady-state preserving operator splitting method and a semi-implicit integration scheme is proposed for efficient time stepping in simulations of unsteady reacting flows, such as turbulent flames, using detailed chemical…

Computational Physics · Physics 2017-12-05 Hao Wu , Peter C. Ma , Matthias Ihme

The evolution of a system of chemical reactions can be studied, in the eikonal approximation, by means of a Hamiltonian dynamical system. The fixed points of this dynamical system represent the different states in which the chemical system…

Statistical Mechanics · Physics 2009-11-13 Carlos Escudero , Jose Angel Rodriguez

Reaction networks in the bulk and on surfaces are widespread in physical, chemical and biological systems. In macroscopic systems, which include large populations of reactive species, stochastic fluctuations are negligible and the reaction…

Statistical Mechanics · Physics 2007-10-12 Baruch Barzel , Ofer Biham , Raz Kupferman

Markov jump processes are continuous-time stochastic processes with a wide range of applications in both natural and social sciences. Despite their widespread use, inference in these models is highly non-trivial and typically proceeds via…

Machine Learning · Computer Science 2023-06-01 Patrick Seifner , Ramses J. Sanchez

A variety of simulation methodologies have been used for modeling reaction-diffusion dynamics -- including approaches based on Differential Equations (DE), the Stochastic Simulation Algorithm (SSA), Brownian Dynamics (BD), Green's Function…

Chemical Physics · Physics 2021-05-21 Marcus Thomas , Russell Schwartz

The simulation of chemical kinetics involving multiple scales constitutes a modeling challenge (from ordinary differential equations to Markov chain) and a computational challenge (multiple scales, large dynamical systems, time step…

Numerical Analysis · Mathematics 2021-06-18 Assyr Abdulle , Lia Gander , Giacomo Rosilho de Souza

Based on a rate equation model for single-mode two-level lasers, two algorithms for stochastically simulating the dynamics and steady-state behaviour of micro- and nanolasers are described in detail. Both methods lead to steady-state photon…

Optics · Physics 2020-10-21 Emil Cortes André , Jesper Mork , Martijn Wubs

Model predictive control strategies require to solve in an sequential manner, many, possibly non-convex, optimization problems. In this work, we propose an interacting stochastic agent system to solve those problems. The agents evolve in…

Optimization and Control · Mathematics 2023-12-21 Giacomo Borghi , Michael Herty

In this paper, we propose a novel sequential data-driven method for dealing with equilibrium based chemical simulations, which can be seen as a specific machine learning approach called active learning. The underlying idea of our approach…

Machine Learning · Statistics 2024-01-26 Mary Savino , Céline Lévy-Leduc , Marc Leconte , Benoit Cochepin

Recently-proposed particle MCMC methods provide a flexible way of performing Bayesian inference for parameters governing stochastic kinetic models defined as Markov (jump) processes (MJPs). Each iteration of the scheme requires an estimate…

Computation · Statistics 2014-05-19 Andrew Golightly , Daniel A. Henderson , Chris Sherlock

At the cellular scale, biochemical processes are governed by random interactions between reactant molecules with small copy counts, leading to behavior that is inherently stochastic. Such systems are often modeled as continuous-time Markov…

Data Structures and Algorithms · Computer Science 2015-09-02 Kevin R. Sanft , Hans G. Othmer

Chemical reactions often proceed through the formation and the consumption of intermediate species. An example is the creation and subsequent degradation of the substrate-enzyme complexes in an enzymatic reaction. In this paper we provide a…

Dynamical Systems · Mathematics 2018-05-22 Daniele Cappelletti , Carsten Wiuf

Sampled structure sequences obtained, for instance, from real-time reactivity explorations or first-principles molecular dynamics simulations contain valuable information about chemical reactivity. Eventually, such sequences allow for the…

Chemical Physics · Physics 2018-04-25 Michael A. Heuer , Alain C. Vaucher , Moritz P. Haag , Markus Reiher

Diffusion mediated reaction models are particularly ubiquitous in the description of physical, chemical or biological processes. The random walk schema is a useful tool for formulating these models. Recently, evanescent random walk models…

Data Analysis, Statistics and Probability · Physics 2015-10-08 Miguel A. Ré , Natalia C. Bustos

We propose a general stochastic formalism for describing the evolution of chemical reactions involving a finite number of molecules. This approach is consistent with the statistical analysis based on the Chemical Master Equation, and…

Statistical Mechanics · Physics 2023-01-13 Chiara Pezzotti , Massimiliano Giona

The goal of the paper is to automatize the selection of mechanisms which are able to describe a set of measurements. In order to do so first we construct a set of possible mechanism fulfilling chemically reasonable requirements with a given…

Numerical Analysis · Mathematics 2019-04-03 Tibor Nagy , János Tóth , Tamás Ladics

A discrete time stochastic model for a multiagent system given in terms of a large collection of interacting Markov chains is studied. The evolution of the interacting particles is described through a time inhomogeneous transition…

Probability · Mathematics 2011-06-17 Amarjit Budhiraja , Pierre Del Moral , Sylvain Rubenthaler