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We present in this paper the main structural features and enthalpy details for the energy profiles of the title reactions, both for the exothermic (forward) path to NH$_{3}$ formation and for the endothermic (reverse) reaction to…

Chemical Physics · Physics 2020-10-30 F. A. Gianturco , E. Yurtsever , M. Satta , R. Wester

The Earth, like other planets with a relatively thick atmosphere, is not locally in radiative equilibrium and the transport of energy by the geophysical fluids (atmosphere and ocean) plays a fundamental role in determining its climate.…

Atmospheric and Oceanic Physics · Physics 2015-05-27 Corentin Herbert , Didier Paillard , Masa Kageyama , Berengere Dubrulle

Minimum energy path (MEP) search is a vital but often very time-consuming method to predict the transition states of versatile dynamic processes in chemistry, physics, and materials science. In this study, we reveal that the chemical bond…

Materials Science · Physics 2023-07-18 Hongsheng Cai , Guoyuan Liu , Peiqi Qiu , Guangfu Luo

Global optimization of transition paths in complex atomic scale systems is addressed in the context of misfit dislocation formation in a strained Ge film on Si(001). Such paths contain multiple intermediate minima connected by minimum…

Materials Science · Physics 2016-06-22 Emile Maras , Oleg Trushin , Alexander Stukowski , Tapio Ala-Nissila , Hannes Jonsson

Finding representative reaction pathways is necessary for understanding mechanisms of molecular processes, but is considered to be extremely challenging. We propose a new method to construct reaction paths based on mean first-passage times.…

Chemical Physics · Physics 2015-06-26 Sanghyun Park , Klaus Schulten

A general method for computing kinetic isotope effects is described. The method uses the quantum-instanton approximation and is based on the thermodynamic integration with respect to the mass of the isotopes and on the path-integral…

Chemical Physics · Physics 2007-05-23 Jiri Vanicek , William H. Miller

Global dynamics in nonlinear stochastic systems is often difficult to analyze rigorously. Yet, many excellent numerical methods exist to approximate these systems. In this work, we propose a method to bridge the gap between computation and…

Dynamical Systems · Mathematics 2019-01-07 Maxime Breden , Christian Kuehn

Simulating transition dynamics between metastable states is a fundamental challenge in dynamical systems and stochastic processes with wide real-world applications in understanding protein folding, chemical reactions and neural activities.…

Machine Learning · Computer Science 2024-10-22 Haibo Wang , Yuxuan Qiu , Yanze Wang , Rob Brekelmans , Yuanqi Du

The quantum instanton approximation is a type of quantum transition state theory that calculates the chemical reaction rate using the reactive flux correlation function and its low order derivatives at time zero. Here we present several…

Chemical Physics · Physics 2009-11-11 Sandy Yang , Takeshi Yamamoto , William H. Miller

In this work, we present a transition-state optimization protocol based on the Mode-Tracking algorithm [J. Chem. Phys. 118 (2003) 1634]. By calculating only the eigenvector of interest instead of diagonalizing the full Hessian matrix and…

Computational Physics · Physics 2015-07-24 Maike Bergeler , Carmen Herrmann , Markus Reiher

We present an information geometric characterization of quantum driving schemes specified by su(2;C) time-dependent Hamiltonians in terms of both complexity and efficiency concepts. By employing a minimum action principle, the optimum path…

Quantum Physics · Physics 2022-04-13 Carlo Cafaro , Shannon Ray , Paul M. Alsing

In coupled rotor models which describe identical rotating nuclei the nuclear spin states restrict the possible angular momenta of each molecule. There are two mean-field approaches to determining the orientational phase diagrams in such…

Statistical Mechanics · Physics 2012-01-13 Balazs Hetenyi

In this paper, we show how the MEP hypothesis may be used to build simple climate models without representing explicitly the energy transport by the atmosphere. The purpose is twofold. First, we assess the performance of the MEP hypothesis…

Atmospheric and Oceanic Physics · Physics 2017-03-21 Corentin Herbert , Didier Paillard

We present a numerical method for computing optimal transition pathways and transition rates in systems of stochastic differential equations (SDEs). In particular, we compute the most probable transition path of stochastic equations by…

Dynamical Systems · Mathematics 2015-06-11 Brandon S. Lindley , Ira B. Schwartz

A general and rigorous methodology to compute the quantum equilibrium isotope effect is described. Unlike standard approaches, ours does not assume separability of rotational and vibrational motions and does not make the harmonic…

Chemical Physics · Physics 2015-05-13 Tomas Zimmermann , Jiri Vanicek

A method for computing minimum ignition energies for gaseous fuel mixtures with detailed and reduced chemistry, by numerical integration of time-dependent conservation equations in a spherically symmetrical configuration, is presented and…

In the framework of a two-moment photo-hydrodynamic modelling of radiation transport, we introduce a concept for the determination of effective radiation transport coefficients based on the minimization of the local entropy production rate…

Statistical Mechanics · Physics 2014-11-18 Thomas Christen , Frank Kassubek

For predicting the kinetics of nucleic acid reactions, continuous-time Markov chains (CTMCs) are widely used. The rate of a reaction can be obtained through the mean first passage time (MFPT) of its CTMC. However, a typical issue in CTMCs…

Quantitative Methods · Quantitative Biology 2021-09-23 Sedigheh Zolaktaf , Frits Dannenberg , Mark Schmidt , Anne Condon , Erik Winfree

Accurate determination of transition states is central to an understanding of reaction kinetics. Double-endpoint methods where both initial and final states are specified, such as the climbing image nudged elastic band (CI-NEB), identify…

Chemical Physics · Physics 2026-04-08 Rohit Goswami , Miha Gunde , Hannes Jónsson

In this article we propose a model based on the Statistical Bootstrap approach to estimate the cross sections of different hadronic reactions up to a few GeV in c.m.s energy. The method is based on the idea, when two particles collide a so…

Nuclear Theory · Physics 2018-04-04 Gábor Balassa , Péter Kovács , György Wolf