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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 present a 3D isotropic ab initio three-body (para-H$_2$)$_3$ interaction potential energy surface (PES). The electronic structure calculations are carried out at the correlated coupled-cluster theory level, with single, double, and…

Chemical Physics · Physics 2025-06-05 Alexander Ibrahim , Pierre-Nicholas Roy

Hydrogen atom transfer (HAT) reactions are essential in many biological processes, such as radical migration in damaged proteins, but their mechanistic pathways remain incompletely understood. Simulating HAT is challenging due to the need…

Machine Learning · Computer Science 2025-11-25 Marlen Neubert , Patrick Reiser , Frauke Gräter , Pascal Friederich

We investigate the endofullerene system $^3$He@C$_{60}$ with a four-dimensional Potential Energy Surface (PES) to include the three He translational degrees of freedom and C$_{60}$ cage radius. We compare MP2, SCS-MP2, SOS-MP2, RPA@PBE and…

Chemical Physics · Physics 2024-03-19 K. Panchagnula , D. Graf , F. E. A. Albertani , A. J. W. Thom

We train an equivariant machine learning model to predict energies and forces for a real-world study of hydrogen combustion under conditions of finite temperature and pressure. This challenging case for reactive chemistry illustrates that…

Chemical Physics · Physics 2023-06-16 Xingyi Guan , Joseph Heindel , Taehee Ko , Chao Yang , Teresa Head-Gordon

We present a first principles-quality potential energy surface (PES) describing the inter-atomic forces for hydrogen atoms interacting with free-standing graphene. The PES is a high-dimensional neural network potential that has been…

The persistence of excitation (PE) condition is sufficient to ensure parameter convergence in adaptive estimation problems. Recent results on adaptive estimation in reproducing kernel Hilbert spaces (RKHS) introduce PE conditions for RKHS.…

Systems and Control · Electrical Eng. & Systems 2020-09-08 Sai Tej Paruchuri , Jia Guo , Andrew Kurdila

Full-dimensional reactive potential energy surfaces (PESs) for the OCS$^+$ cation are constructed to describe S$^+$ loss in the electronic ground state and seven low-lying electronically excited states. High-level \textit{ab initio}…

Chemical Physics · Physics 2026-05-15 Cangtao Yin , Stefan Willitsch , Markus Meuwly

There has been a veritable explosion of methods and software to perform machine-learned regression on datasets of electronic energies and forces to develop high-dimensional machine learned potential energy surfaces (ML-PESs). A major, but…

Ring polymer molecular dynamics (RPMD) has proven to be an accurate approach for calculating thermal rate coefficients of various chemical reactions. For wider application of this methodology, efficient ways to generate the underlying…

Chemical Physics · Physics 2020-01-08 Ivan S. Novikov , Alexander V. Shapeev , Yury V. Suleimanov

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

We present an exhaustive study of more than 250 ab initio potential energy surfaces (PESs) of the model dipeptide HCO-L-Ala-NH2. The model chemistries (MCs) used are constructed as homo- and heterolevels involving possibly different RHF and…

Quantitative Methods · Quantitative Biology 2013-06-21 Pablo Echenique , J. L. Alonso

We show that chemically-accurate potential energy surfaces (PESs) can be generated from quantum computers by measuring only the density along an adiabatic transition between different molecular geometries. In lieu of using phase estimation,…

Quantum Physics · Physics 2024-10-08 James Brown

Accurate, global Potential Energy Surfaces (PES) expressed in sum-of-products (SOP) form are a prerequisite for efficient high-dimensional quantum dynamics simulations using the MCTDH method. This work introduces a methodology for…

Chemical Physics · Physics 2026-03-31 Antoine Aerts

Full dimensional potential energy surfaces (PESs) based on machine learning (ML) techniques provide means for accurate and efficient molecular simulations in the gas- and condensed-phase for various experimental observables ranging from…

Chemical Physics · Physics 2023-07-26 Kaisheng Song , Silvan Käser , Kai Töpfer , Luis Itza Vazquez-Salazar , Markus Meuwly

Machine learning models are changing the paradigm of molecular modeling, which is a fundamental tool for material science, chemistry, and computational biology. Of particular interest is the inter-atomic potential energy surface (PES). Here…

Computational Physics · Physics 2020-07-21 Linfeng Zhang , Jiequn Han , Han Wang , Wissam A. Saidi , Roberto Car , Weinan E

We present an isotropic ab initio (para-H$_2$)$_4$ four-body interaction potential energy surface (PES). The electronic structure calculations are performed at the correlated coupled-cluster theory level, with single, double, and…

Chemical Physics · Physics 2025-06-09 Alexander Ibrahim , Pierre-Nicholas Roy

The rise of machine learning has greatly influenced the field of computational chemistry, and that of atomistic molecular dynamics simulations in particular. One of its most exciting prospects is the development of accurate,…

Chemical Physics · Physics 2023-06-14 Silvan Käser , Markus Meuwly

Permutationally invariant polynomial (PIP) regression has been used to obtain machine-learned (ML) potential energy surfaces, including analytical gradients, for many molecules and chemical reactions. Recently, the approach has been…

Chemical Physics · Physics 2024-07-30 Paul L. Houston , Chen Qu , Apurba Nandi , Riccardo Conte , Qi Yu , Joel M. Bowman

In order to predict the potential energy surface (PES) from measured structure in equilibrium state, one should typically perform trial-and-error statistical thermodynamic simulation with assumed multibody interactions. Very recently, we…

Disordered Systems and Neural Networks · Physics 2017-07-11 Koretaka Yuge