Amb motiu del tancament d'estiu, la validació de documents es reprendrà a partir del 28 d'agost de 2026. Disculpeu les molèsties.
Con motivo del cierre de verano, la validación de documentos se reanudará a partir del 28 de agosto de 2026. Disculpad las molestias
Due to the summer closure, document validation will resume starting August 28, 2026. We apologize for any inconvenience.

Files

674247.pdf (8.65 MB)

Document type

Article

Version

Published version

Publication date

2017-08-01

All rights reserved

Please use this identifier to cite or link to this item: https://hdl.handle.net/2445/122412

An algorithm to locate optimal bond breaking points on a potential energy surface for applications in mechanochemistry and catalysis

Journal Title

Authors

Director/Tutor

Journal ISSN

Volume Title

Related resource

https://doi.org/10.1063/1.4994925

Abstract

The reaction path of a mechanically induced chemical transformation changes under stress. It is well established that the force-induced structural changes of minima and saddle points, i.e., the movement of the stationary points on the original or stress-free potential energy surface, can be described by a Newton Trajectory (NT). Given a reactive molecular system, a well-fitted pulling direction, and a sufficiently large value of the force, the minimum configuration of the reactant and the saddle point configuration of a transition state collapse at a point on the corresponding NT trajectory. This point is called barrier breakdown point or bond breaking point (BBP). The Hessian matrix at the BBP has a zero eigenvector which coincides with the gradient. It indicates which force (both in magnitude and direction) should be applied to the system to induce the reaction in a barrierless process. Within the manifold of BBPs, there exist optimal BBPs which indicate what is the optimal pulling direction and what is the minimal magnitude of the force to be applied for a given mechanochemical transformation. Since these special points are very important in the context of mechanochemistry and catalysis, it is crucial to develop efficient algorithms for their location. Here, we propose a Gauss-Newton algorithm that is based on the minimization of a positively defined function (the so-called -function). The behavior and efficiency of the new algorithm are shown for 2D test functions and for a real chemical example.

Subject

Algorismes, Catàlisi

Subject (English)

Algorithms, Catalysis

Citation

Collections

Articles publicats en revistes (Química Inorgànica i Orgànica)
Articles publicats en revistes (Ciència dels Materials i Química Física)
Articles publicats en revistes (Institut de Química Teòrica i Computacional (IQTCUB))

Citation

BOFILL I VILLÀ, Josep M., et al. An algorithm to locate optimal bond breaking points on a potential energy surface for applications in mechanochemistry and catalysis. Journal of Chemical Physics. 2017. Vol. 147, num. 15, pags. 152710-1-152710-10. ISSN 0021-9606. [consulted: 15 of August of 2026]. Available at: https://hdl.handle.net/2445/122412

Export metadata

JSON - METS

Share record