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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 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

Understanding and accurately predicting hydrogen diffusion in materials is challenging due to the complex interactions between hydrogen defects and the crystal lattice. These interactions span large length and time scales, making them…

This paper concerns the use of the expectation-maximisation (EM) algorithm for inference in partially observed diffusion processes. In this context, a well known problem is that all except a few diffusion processes lack closed-form…

Statistics Theory · Mathematics 2010-08-18 Jimmy Olsson , Jonas Ströjby

In this work, we present Enhanced Representation-Based Sampling (ERBS), a novel enhanced sampling method designed to generate structurally diverse training datasets for machine-learned interatomic potentials. ERBS automatically identifies…

Chemical Physics · Physics 2026-01-23 Moritz René Schäfer , Johannes Kästner

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

Machine learning assisted modeling of the inter-atomic potential energy surface (PES) is revolutionizing the field of molecular simulation. With the accumulation of high-quality electronic structure data, a model that can be pretrained on…

Chemical Physics · Physics 2023-09-18 Duo Zhang , Hangrui Bi , Fu-Zhi Dai , Wanrun Jiang , Linfeng Zhang , Han Wang

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 elementary excitations in metallic glasses (MGs), i.e., $\beta$ processes that involve hopping between nearby sub-basins, underlie many unusual properties of the amorphous alloys. A high-efficacy prediction of the propensity for those…

Materials Science · Physics 2020-06-25 Qi Wang , Jun Ding , Evan Ma

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

Despite the widespread use of Scanning Transmission Electron Microscopy (STEM) for observing the structure of materials at the atomic scale, a detailed understanding of some relevant electron beam damage mechanisms is limited. Recent…

Limited by the encoder-decoder architecture, learning-based edge detectors usually have difficulty predicting edge maps that satisfy both correctness and crispness. With the recent success of the diffusion probabilistic model (DPM), we…

Computer Vision and Pattern Recognition · Computer Science 2024-01-10 Yunfan Ye , Kai Xu , Yuhang Huang , Renjiao Yi , Zhiping Cai

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…

While energy-based models (EBMs) exhibit a number of desirable properties, training and sampling on high-dimensional datasets remains challenging. Inspired by recent progress on diffusion probabilistic models, we present a diffusion…

Machine Learning · Computer Science 2021-03-30 Ruiqi Gao , Yang Song , Ben Poole , Ying Nian Wu , Diederik P. Kingma

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…

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

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

Atmospheric moist available potential energy (MAPE) has been traditionally defined as the potential energy of a moist atmosphere relative to that of the adiabatically sorted reference state defining a global potential energy minimum.…

Atmospheric and Oceanic Physics · Physics 2018-11-14 Bethan L. Harris , Remi Tailleux

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

Electron density is a fundamental quantity, which can in principle determine all ground state electronic properties of a given system. Although machine learning (ML) models for electron density based on either an atom-centered basis or a…

Chemical Physics · Physics 2024-10-08 Chaoqiang Feng , Yaolong Zhang , Bin Jiang