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Machine learning of multi-dimensional potential energy surfaces, from purely ab initio datasets, has seen substantial progress in the past years. Gaussian processes, a popular regression method, have been very successful at producing…

Chemical Physics · Physics 2023-01-11 Fabio E. A. Albertani , Alex J. W. Thom

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

In this work, we propose a multi-scale protocol for routine theoretical studies of chemical reaction mechanisms. The initial reaction paths of our investigated systems are sampled using the Nudged-Elastic Band (NEB) method driven by a cheap…

Chemical Physics · Physics 2023-07-26 Tomislav Piskor , Peter Pinski , Thilo Mast , Vladimir V. Rybkin

The predictive simulation of molecular liquids requires models that are not only accurate, but computationally efficient enough to handle the large systems and long time scales required for reliable prediction of macroscopic properties. We…

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 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

The variational quantum eigensolver (or VQE) uses the variational principle to compute the ground state energy of a Hamiltonian, a problem that is central to quantum chemistry and condensed matter physics. Conventional computing methods are…

We present a simple, yet general, end-to-end deep neural network representation of the potential energy surface for atomic and molecular systems. This methodology, which we call Deep Potential, is "first-principle" based, in the sense that…

Computational Physics · Physics 2020-07-20 Jiequn Han , Linfeng Zhang , Roberto Car , Weinan E

Kernel models of potential energy surfaces (PES) for polyatomic molecules are often restricted by a specific choice of the kernel function. This can be avoided by optimizing the complexity of the kernel function. For regression problems…

Chemical Physics · Physics 2023-05-02 Jun Dai , Roman V. Krems

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

The exploration of molecular systems' potential energy surface is important for comprehending their complex behaviors, particularly through identifying various metastable states. However, the transition between these states is often…

Chemical Physics · Physics 2024-04-05 Janghoon Ock , Parisa Mollaei , Amir Barati Farimani

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 process of design and discovery of new materials can be significantly expedited and simplified if we can learn effectively from available data. Deep learning (DL) approaches have recently received a lot of interest for their ability to…

Progress in machine learning has facilitated the development of potentials that offer both the accuracy of first-principles techniques and vast increases in the speed of evaluation. Recently,"$\Delta$-machine learning" has been used to…

Current quantum computers are limited in the number of qubits and coherence time, constraining the algorithms executable with sufficient fidelity. The variational quantum eigensolver (VQE) is an algorithm to find an approximate ground state…

Quantum Physics · Physics 2023-01-24 Luca Erhart , Kosuke Mitarai , Wataru Mizukami , Keisuke Fujii

Machine learned interatomic potentials (MLIPs) are becoming a standard method for DFT-level accurate molecular dynamics simulation and large-scale studies of crystal energetics. Increasingly popular are universal pre-trained potentials,…

Materials Science · Physics 2026-02-03 Abhijith S Parackal , Rickard Armiento , Florian Trybel

A neural network-based machine learning potential energy surface (PES) expressed in a matrix product operator (NN-MPO) is proposed. The MPO form enables efficient evaluation of high-dimensional integrals that arise in solving the…

Machine Learning · Computer Science 2025-05-07 Kentaro Hino , Yuki Kurashige

A very accurate, (HF)$_2$ potential energy surface (PES) due to Huang et al. (J. Chem. Phys., 150, 154302 (2019)) is used to calculate the energy levels of the HF dimer by solving the nuclear-motion Schr\"{o}dinger equation using…

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

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