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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

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

Gaussian process regression has recently emerged as a powerful, system-agnostic tool for building global potential energy surfaces (PES) of polyatomic molecules. While the accuracy of GP models of PES increases with the number of potential…

Chemical Physics · Physics 2019-07-23 Jun Dai , Roman V. Krems

A new nine-dimensional potential energy surface (PES) for methane has been generated using state-of-the-art \textit{ab initio} theory. The PES is based on explicitly correlated coupled cluster calculations with extrapolation to the complete…

Chemical Physics · Physics 2016-10-12 Alec Owens , Sergey N. Yurchenko , Andrey Yachmenev , Jonathan Tennyson , Walter Thiel

The idea of a Potential Energy Surface (PES) forms the basis of almost all accounts of the mechanisms of chemical reactions, and much of theoretical molecular spectroscopy. It is assumed that, in principle, the PES can be calculated by…

Quantum Physics · Physics 2013-04-10 Brian Sutcliffe , R. Guy Woolley

An overview of computational methods to describe high-dimensional potential energy surfaces suitable for atomistic simulations is given. Particular emphasis is put on accuracy, computability, transferability and extensibility of the methods…

Chemical Physics · Physics 2020-07-08 Oliver T. Unke , Debasish Koner , Sarbani Patra , Silvan Käser , Markus Meuwly

The potential energy surface (PES) is crucial for interpreting a variety of chemical reaction processes. However, predicting accurate PESs with high-level electronic structure methods is a challenging task due to the high computational…

Chemical Physics · Physics 2022-06-09 Yanxian Tao , Xiongzhi Zeng , Yi Fan , Jie Liu , Zhenyu Li , Jinlong Yang

Atomistic simulations are a powerful tool for studying the dynamics of molecules, proteins, and materials on wide time and length scales. Their reliability and predictiveness, however, depend directly on the accuracy of the underlying…

Chemical Physics · Physics 2024-11-28 Silvan Käser , Debasish Koner , Markus Meuwly

We explore the performance of a statistical learning technique based on Gaussian Process (GP) regression as an efficient non-parametric method for constructing multi-dimensional potential energy surfaces (PES) for polyatomic molecules.…

Chemical Physics · Physics 2016-11-23 Jie Cui , Roman V. Krems

A new nine-dimensional potential energy surface (PES) and dipole moment surface (DMS) for silane have been generated using high-level \textit{ab initio} theory. The PES, CBS-F12$^{\,\mathrm{HL}}$, reproduces all four fundamental term values…

Chemical Physics · Physics 2018-08-17 Alec Owens , Sergei N. Yurchenko , Andrey Yachmenev , Walter Thiel

The interpolation of high-dimensional potential energy surfaces (PESs) is commonly done with physically-inspired deep-neural network models. In this work, we illustrate that Gaussian Processes (GPs) are also capable of interpolating…

Chemical Physics · Physics 2021-09-30 Rodrigo A. Vargas-Hernández , Jake R. Gardner

The accurate description of molecule-surface interactions requires a detailed knowledge of the underlying potential-energy surface (PES). Recently, neural networks (NNs) have been shown to be an efficient technique to accurately interpolate…

Materials Science · Physics 2009-11-13 Jorg Behler , Sonke Lorenz , Karsten Reuter

Transition intensities for small molecules such as water and CO$_2$ can now be computed with such high accuracy that they are being used to systematically replace measurements in standard databases. These calculations use high accuracy ab…

We present an efficient approach for generating highly accurate molecular potential energy surfaces (PESs) using self-correcting, kernel ridge regression (KRR) based machine learning (ML). We introduce structure-based sampling to…

Chemical Physics · Physics 2018-08-20 Pavlo O. Dral , Alec Owens , Sergei N. Yurchenko , Walter Thiel

The construction of the potential energy surface (PES) of even a medium-sized molecule employing correlated theory, such as CCSD(T), is an arduous task due to the high computational cost. In this Letter, we report the possibility of…

Chemical Physics · Physics 2022-05-04 Subodh S. Khire , Nalini D. Gurav , Apurba Nandi , Shridhar R. Gadre

Machine-learned potential energy surfaces (PESs) for molecules with more than 10 atoms are typically forced to use lower-level electronic structure methods such as density functional theory and second-order Moller-Plesset perturbation…

Chemical Physics · Physics 2021-05-21 Chen Qu , Paul Houston , Riccardo Conte , Apurba Nandi , Joel M. Bowman

We propose a machine-learning approach based on Bayesian optimization to build global potential energy surfaces (PES) for reactive molecular systems using feedback from quantum scattering calculations. The method is designed to correct for…

Chemical Physics · Physics 2019-03-27 R. A. Vargas-Hernández , Y. Guan , D. H. Zhang , R. V. Krems

Potential Energy Surfaces (PESs) are an indispensable tool to investigate, characterise and understand chemical and biological systems in the gas and condensed phases. Advances in Machine Learning (ML) methodologies have led to the…

Chemical Physics · Physics 2025-11-04 Valerii Andreichev , Sena Aydin , Kai Töpfer , Markus Meuwly , Luis Itza Vazquez-Salazar

The interaction potential energy surface (PES) of He-H2 is of great importance for quantum chemistry, as the simplest test case for interactions between a molecule and a closed-shell atom. It is also required for a detailed understanding of…

Astrophysics · Physics 2009-11-07 Arnold I. Boothroyd , Peter G. Martin , Michael R. Peterson

We investigate the endofullerene system Ne@C$_{70}$, by constructing a three-dimensional Potential Energy Surface (PES) describing the translational motion of the Ne atom. We compare a plethora of electronic structure methods including:…

Chemical Physics · Physics 2024-06-12 K. Panchagnula , D. Graf , E. R. Johnson , A. J. W. Thom
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