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With gates of a quantum computer designed to encode multi-dimensional vectors, projections of quantum computer states onto specific qubit states can produce kernels of reproducing kernel Hilbert spaces. We show that quantum kernels obtained…

Quantum Physics · Physics 2024-06-19 Jun Dai , Roman V. Krems

An efficient and trajectory-free active learning method is proposed to automatically sample data points for constructing globally accurate reactive potential energy surfaces (PESs) using neural networks (NNs). Although NNs do not provide…

Chemical Physics · Physics 2020-05-20 Qidong Lin , Yaolong Zhang , Bin Zhao , Bin Jiang

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 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

The potential energy surface (PES) of molecules with respect to their nuclear positions is a primary tool in understanding chemical reactions from first principles. However, obtaining this information is complicated by the fact that…

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

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

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

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

We show that a Gaussian Process model can be combined with a small number (of order 100) of scattering calculations to provide a multi-dimensional dependence of scattering observables on the experimentally controllable parameters such as…

Chemical Physics · Physics 2015-08-19 Jie Cui , Roman V. Krems

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

We propose a novel information-theoretic approach for Bayesian optimization called Predictive Entropy Search (PES). At each iteration, PES selects the next evaluation point that maximizes the expected information gained with respect to the…

Machine Learning · Statistics 2014-06-11 José Miguel Hernández-Lobato , Matthew W. Hoffman , Zoubin Ghahramani

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 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 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

Constructing accurate, high dimensional molecular potential energy surfaces (PESs) for polyatomic molecules is challenging. Reproducing Kernel Hilbert space (RKHS) interpolation is an efficient way to construct such PESs. However, the…

Chemical Physics · Physics 2020-11-06 Debasish Koner , Markus Meuwly

Computational chemistry has become an important tool to predict and understand molecular properties and reactions. Even though recent years have seen a significant growth in new algorithms and computational methods that speed up quantum…

Chemical Physics · Physics 2023-07-26 Albert Thie , Maximilian F. S. J. Menger , Shirin Faraji

We investigate a novel stochastic technique for the global optimization of complex potential energy surfaces (PES) that avoids the freezing problem of simulated annealing by allowing the dynamical process to tunnel energetically…

Computational Physics · Physics 2009-10-31 W. Wenzel , K. Hamacher

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

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
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