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Accurate potential energy surfaces (PESs) have been determined for the $^3$A$'$ and $^3$A$''$ states of N$_2$O using electronic structure calculations at the multireference configuration interaction level with Davidson correction (MRCI+Q)…

Chemical Physics · Physics 2020-11-06 Debasish Koner , Juan Carlos San Vicente Veliz , Raymond J. Bemish , Markus Meuwly

Characterizing conformational transitions in physical systems remains a fundamental challenge, as traditional sampling methods struggle with the high-dimensional nature of molecular systems and high-energy barriers between stable states.…

Chemical Physics · Physics 2025-09-22 Magnus Petersen , Gemma Roig , Roberto Covino

Transition state (TS) searches are a critical bottleneck in computational studies of chemical reactivity, as accurately capturing complex phenomena like bond breaking and formation events requires repeated evaluations of expensive ab-initio…

Chemical Physics · Physics 2025-09-23 Jonah Marks , Joseph Gomes

Free energy profile (FE Profile) is an essential quantity for the estimation of reaction rate and the validation of reaction mechanism. For chemical reactions in condensed phase or enzymatic reactions, the computation of FE profile at ab…

Computational Physics · Physics 2018-11-15 Pengfei Li , Xiangyu Jia , Xiaoliang Pan , Yihan Shao , Ye Mei

Non-adiabatic effects play an important role in many chemical processes. In order to study the underlying non-adiabatic potential-energy surfaces (PESs), we present a locally-constrained density-functional theory approach, which enables us…

Materials Science · Physics 2015-06-25 Joerg Behler , Bernard Delley , Karsten Reuter , Matthias Scheffler

We propose a method that exploits sparse representation of potential energy surfaces (PES) on a polynomial basis set selected by compressed sensing. The method is useful for studies involving large numbers of PES evaluations, such as the…

Chemical Physics · Physics 2018-08-10 Prashant Rai , Khachik Sargsyan , Habib Najm , So Hirata

Low-loss electron energy loss spectroscopy (EELS) has emerged as a technique of choice for exploring the localization of plasmonic phenomena at the nanometer level, necessitating analysis of physical behaviors from 3D spectral data sets.…

Chemical selectivity, as quantified by a branching ratio, is a phenomenon relevant for many organic chemical reactions. It may be exhibited on a potential energy surface that features a valley-ridge inflection point in the region between…

Chemical Physics · Physics 2020-08-26 V. J. García-Garrido , M. Katsanikas , M. Agaoglou , S. Wiggins

The alignment of the frontier orbital energies of an adsorbed molecule with the substrate Fermi level at metal-organic interfaces is a fundamental observable of significant practical importance in nanoscience and beyond. Typical density…

Mesoscale and Nanoscale Physics · Physics 2017-03-07 Zhenfei Liu , David A. Egger , Sivan Refaely-Abramson , Leeor Kronik , Jeffrey B. Neaton

The goal of the present work is to obtain accurate potential energy surfaces (PES) for high-dimensional molecular systems with a small number of ${\it ab}$ ${\it initio}$ calculations in a system-agnostic way. We use probabilistic modeling…

Computational Physics · Physics 2020-08-27 Hiroki Sugisawa , Tomonori Ida , Roman V. Krems

The structure and dynamics of a molecular system is governed by its potential energy surface (PES), representing the total energy as a function of the nuclear coordinates. Obtaining accurate potential energy surfaces is limited by the…

Chemical Physics · Physics 2023-09-29 Karl P. Horn , Luis Itza Vazquez-Salazar , Christiane P. Koch , Markus Meuwly

Machine Learning techniques can be used to represent high-dimensional potential energy surfaces for reactive chemical systems. Two such methods are based on a reproducing kernel Hilbert space representation or on deep neural networks. They…

Chemical Physics · Physics 2019-09-19 Oliver T. Unke , Markus Meuwly

We compare the predicted phase behaviour of lead (Pb) using three different interatomic potential models, including an embedded atom method (EAM), a modified embedded atom method (MEAM), and a neural network-based machine-learned model in…

Simulating interactions between non-spherical colloidal particles is computationally challenging due to the complex dependency of forces and energies on their geometry. We introduce and evaluate both descriptor-based and end-to-end models…

Soft Condensed Matter · Physics 2025-09-22 B. Rusen Argun , Antonia Statt

The atom-exchange and atomization dissociation dynamics for the N($^4$S) + N$_2(^1 \Sigma_{\rm g}^+)$ reaction is studied using a reproducing kernel Hilbert space (RKHS)-based, global potential energy surface (PES) at the…

Chemical Physics · Physics 2024-04-30 JingChun Wang , Juan Carlos San Vicente Veliz , Markus Meuwly

Given a chemical reaction going from reactant (R) to the product (P) on a potential energy surface (PES) and a collective variable (CV) that discriminates between R and P, one can define a free-energy profile (FEP) as the logarithm of the…

Mapping reaction pathways and transition states (TS) is fundamental to chemistry but computationally expensive at scale. The minimum energy pathway (MEP) dictates reaction rates and mechanisms, yet recovering it via electronic-structure…

Chemical Physics · Physics 2026-05-25 Rémi Schlama , Philippe Schwaller

In reaction path optimization, such as the calculation of a minimum energy path (MEP) between given reactant and product configurations of atoms, it is advantageous to start with an initial guess where close proximity of atoms is avoided…

Chemical Physics · Physics 2023-10-10 Yorick L. A. Schmerwitz , Vilhjálmur Ásgeirsson , Hannes Jónsson

High-quality potential energy surfaces (PES) are a prerequisite for quantitative atomistic simulations, with both quantum and classical dynamics approaches. The ultimate test for the validity of a PES are comparisons with judiciously chosen…