Related papers: Phase-space resolved rates in driven multidimensio…
Reaction rates of chemical reactions under nonequilibrium conditions can be determined through the construction of the normally hyperbolic invariant manifold (NHIM) [and moving dividing surface (DS)] associated with the transition state…
The rate of a chemical reaction can often be determined by the properties of a rank-1 saddle and the associated transition state separating reactants and products. We have found evidence that such rates can be controlled and even enhanced…
Recent work has shown that in a non-thermal, multidimensional system, the trajectories in the activated complex possess different instantaneous and time-averaged reactant decay rates. Under dissipative dynamics, it is known that these…
Chemical reactions in multidimensional systems are often described by a rank-1 saddle, whose stable and unstable manifolds intersect in the normally hyperbolic invariant manifold (NHIM). Trajectories started on the NHIM in principle never…
The identification of trajectories that contribute to the reaction rate is the crucial dynamical ingredient in any classical chemical reactivity calculation. This problem often requires a full scale numerical simulation of the dynamics, in…
Computing accurate rate constants for catalytic events occurring at the surface of a given material represents a challenging task with multiple potential applications in chemistry. To address this question, we propose an approach based on a…
We study the phase space geometry associated with index 2 saddles of a potential energy surface and its influence on reaction dynamics for $n$ degree-of-freedom (DoF) Hamiltonian systems. For index 1 saddles of potential energy surfaces…
We consider the existence of invariant manifolds in phase space governing reaction dynamics in situations where there are no saddle points on the potential energy surface in the relevant regions of configuration space. We point out that…
A model Hamiltonian for the reaction CH$_4^+ \rightarrow$ CH$_3^+$ + H, parametrized to exhibit either early or late inner transition states, is employed to investigate the dynamical characteristics of the roaming mechanism. Tight/loose…
The framework of transition state theory (TST) provides a powerful way for analyzing the dynamics of physical and chemical reactions. While TST has already been successfully used to obtain reaction rates for systems with a single…
Common modal decomposition techniques for flowfield analysis, data-driven modeling and flow control, such as proper orthogonal decomposition (POD) and dynamic mode decomposition (DMD) are usually performed in an Eulerian (fixed) frame of…
Ab initio molecular dynamics (AIMD) based on density functional theory (DFT) has become a workhorse for studying the structure, dynamics, and reactions in condensed matter systems. Currently, AIMD simulations are primarily carried out at…
We present a fully adaptive multiresolution scheme for spatially two-dimensional, possibly degenerate reaction-diffusion systems, focusing on combustion models and models of pattern formation and chemotaxis in mathematical biology.…
Hamiltonian dynamical systems possessing equilibria of ${saddle} \times {centre} \times...\times {centre}$ stability type display \emph{reaction-type dynamics} for energies close to the energy of such equilibria; entrance and exit from…
We present a new method for the numerical calculation of canonical reaction rate constants in complex molecular systems, which is based on a path integral formulation of the flux-flux correlation function. Central is the partitioning of the…
Contemporary materials science research is heavily conducted in silico, involving massive simulations of the atomic-scale evolution of materials. Cataloging basic patterns in the atomic displacements is key to understanding and predicting…
Computing reaction rates in biomolecular systems is a common goal of molecular dynamics simulations. The reactions considered often involve conformational changes in the molecule, either changes in the structure of a protein or the relative…
In many reacting flow systems, the thermo-chemical state-space is known or assumed to evolve close to a low-dimensional manifold (LDM). Various approaches are available to obtain those manifolds and subsequently express the original…
A dilute system of reacting particles transported by fluid flows is considered. The particles react as $A + A \to \varnothing$ with a given rate when they are within a finite radius of interaction. The system is described in terms of the…
This article concerns two methods for reducing large systems of chemical kinetics equations, namely, the method of intrinsic low-dimensional manifolds (ILDMs) due to Maas and Pope and an iterative method due to Fraser and further developed…