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Machine Learning (ML) has become a promising tool for improving the quality of atomistic simulations. Using formaldehyde as a benchmark system for intramolecular interactions, a comparative assessment of ML models based on state-of-the-art…

Conventional kernel-based machine learning models for ab initio potential energy surfaces, while accurate and convenient in small data regimes, suffer immense computational cost as training set sizes increase. We introduce QML-Lightning, a…

Chemical Physics · Physics 2022-12-21 Nicholas J. Browning , Felix A. Faber , O. Anatole von Lilienfeld

The answers to many unsolved problems lie in the intractable chemical space of molecules and materials. Machine learning techniques are rapidly growing in popularity as a way to compress and explore chemical space efficiently. One of the…

Chemical Physics · Physics 2020-01-06 John E. Herr , Kevin Koh , Kun Yao , John Parkhill

We introduce an unsupervised clustering algorithm to improve training efficiency and accuracy in predicting energies using molecular-orbital-based machine learning (MOB-ML). This work determines clusters via the Gaussian mixture model (GMM)…

Chemical Physics · Physics 2023-03-28 Lixue Cheng , Jiace Sun , Thomas F. Miller

Modern machine learning (ML) models of chemical and materials systems with billions of parameters require vast training datasets and considerable computational efforts. Lightweight kernel or decision tree based methods, however, can be…

Chemical Physics · Physics 2024-10-18 Danish Khan , O. Anatole von Lilienfeld

We show how machine learning techniques based on Bayesian inference can be used to reach new levels of realism in the computer simulation of molecular materials, focusing here on water. We train our machine-learning algorithm using…

Materials Science · Physics 2013-02-25 Albert P. Bartok , Michael J. Gillan , Frederick R. Manby , Gabor Csanyi

Recently, machine learning Hamiltonian (MLH) models have gained traction as fast approximations of electronic structures such as orbitals and electron densities, while also enabling direct evaluation of energies and forces from their…

We present a scheme to obtain an inexpensive and reliable estimate of the uncertainty associated with the predictions of a machine-learning model of atomic and molecular properties. The scheme is based on resampling, with multiple models…

Chemical Physics · Physics 2025-10-06 Felix Musil , Michael J. Willatt , Mikhail A. Langovoy , Michele Ceriotti

Energy functions for pure and heterogenous systems are one of the backbones for molecular simulation of condensed phase systems. With the advent of machine learned potential energy surfaces (ML-PESs) a new era has started. Statistical…

We introduce machine learning models of quantum mechanical observables of atoms in molecules. Instant out-of-sample predictions for proton and carbon nuclear chemical shifts, atomic core level excitations, and forces on atoms reach…

Chemical Physics · Physics 2015-08-26 Matthias Rupp , Raghunathan Ramakrishnan , O. Anatole von Lilienfeld

Quantum mechanics/molecular mechanics (QM/MM) molecular dynamics (MD) simulations have been developed to simulate molecular systems, where an explicit description of changes in the electronic structure is necessary. However, QM/MM MD…

Chemical Physics · Physics 2021-04-15 Lennard Böselt , Moritz Thürlemann , Sereina Riniker

Free energies govern the behavior of soft and liquid matter, and improving their predictions could have a large impact on the development of drugs, electrolytes or homogeneous catalysts. Unfortunately, it is challenging to devise an…

Chemical Physics · Physics 2021-04-14 Jan Weinreich , Nicholas J. Browning , O. Anatole von Lilienfeld

We introduce a local machine-learning method for predicting the electron densities of periodic systems. The framework is based on a numerical, atom-centred auxiliary basis, which enables an accurate expansion of the all-electron density in…

Chemical Physics · Physics 2021-11-10 Alan M. Lewis , Andrea Grisafi , Michele Ceriotti , Mariana Rossi

Process optimization in chemical engineering may be hindered by the limited availability of reliable thermodynamic data for fluid mixtures. Remarkable progress is being made in predicting thermodynamic mixture properties by machine learning…

Computational Engineering, Finance, and Science · Computer Science 2025-10-14 Martin Bubel , Tobias Seidel , Michael Bortz

Machine learning (ML) provides access to fast and accurate quantum chemistry (QC) calculations for various properties of interest such as excitation energies. It is often the case that high accuracy in prediction using an ML model, demands…

Chemical Physics · Physics 2024-03-13 Vivin Vinod , Ulrich Kleinekathöfer , Peter Zaspel

Machine Learning algorithms based on Brain-inspired Hyperdimensional(HD) computing imitate cognition by exploiting statistical properties of high-dimensional vector spaces. It is a promising solution for achieving high energy efficiency in…

Machine Learning · Computer Science 2022-10-12 Samuel Bosch , Alexander Sanchez de la Cerda , Mohsen Imani , Tajana Simunic Rosing , Giovanni De Micheli

Accumulation of molecular data obtained from quantum mechanics (QM) theories such as density functional theory (DFTQM) make it possible for machine learning (ML) to accelerate the discovery of new molecules, drugs, and materials. Models…

Chemical Physics · Physics 2020-11-04 Alain B. Tchagang , Ahmed H. Tewfik , Julio J. Valdés

Aerosol particles play an important role in the climate system by absorbing and scattering radiation and influencing cloud properties. They are also one of the biggest sources of uncertainty for climate modeling. Many climate models do not…

Machine Learning · Computer Science 2021-09-30 Paula Harder , Duncan Watson-Parris , Dominik Strassel , Nicolas Gauger , Philip Stier , Janis Keuper

The ability to perform ab initio molecular dynamics simulations using potential energies calculated on quantum computers would allow virtually exact dynamics for chemical and biochemical systems, with substantial impacts on the fields of…

Abstract Machine learning models, trained on data from ab initio quantum simulations, are yielding molecular dynamics potentials with unprecedented accuracy. One limiting factor is the quantity of available training data, which can be…

Computational Physics · Physics 2020-06-11 Justin S. Smith , Nicholas Lubbers , Aidan P. Thompson , Kipton Barros
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