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Related papers: Adaptive atomic basis sets

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Strong magnetic fields such as those found on white dwarfs have significant effects on the electronic structure of atoms and molecules. However, the vast majority of molecular studies in the literature in such fields are carried out with…

Chemical Physics · Physics 2025-02-07 Hugo Åström , Susi Lehtola

Quantum Computing (QC) offers outstanding potential for molecular characterization and drug discovery, particularly in solving complex properties like the Ground State Energy (GSE) of biomolecules. However, QC faces challenges due to…

Chemical Physics · Physics 2024-12-17 Laia Coronas Sala , Parfait Atchade-Adelemou

Uncertainty control and scalability to large datasets are the two main issues for the deployment of Gaussian process (GP) models within the autonomous machine learning-based prediction pipelines in material science and chemistry. One way to…

Chemical Physics · Physics 2024-02-21 Mikhail Tsitsvero , Mingoo Jin , Andrey Lyalin

Classical empirical force fields have dominated biomolecular simulation for over 50 years. Although widely used in drug discovery, crystal structure prediction, and biomolecular dynamics, they generally lack the accuracy and transferability…

This study extends the accurate and transferable molecular-orbital-based machine learning (MOB-ML) approach to modeling the contribution of electron correlation to dipole moments at the cost of Hartree-Fock computations. A…

Chemical Physics · Physics 2022-09-21 Jiace Sun , Lixue Cheng , Thomas F. Miller

Data-driven, machine learning (ML) models of atomistic interactions are often based on flexible and non-physical functions that can relate nuanced aspects of atomic arrangements into predictions of energies and forces. As a result, these…

Materials Science · Physics 2024-05-15 Bartosz Barzdajn , Christopher P. Race

With the recent advances in the development of devices capable of performing quantum computations, a growing interest in finding near-term applications has emerged in many areas of science. In the era of non-fault tolerant quantum devices,…

Universal machine-learned interatomic potentials (U-MLIPs) have demonstrated effectiveness across diverse atomistic systems but often require fine-tuning for task-specific accuracy. We investigate the fine-tuning of two MACE-based…

Computational Physics · Physics 2025-06-10 Xiaoqing Liu , Kehan Zeng , Yangshuai Wang , Teng Zhao

Molecular dynamics simulations are an invaluable tool in numerous scientific fields. However, the ubiquitous classical force fields cannot describe reactive systems, and quantum molecular dynamics are too computationally demanding to treat…

Chemical Physics · Physics 2022-08-09 Xiangyun Lei , Andrew J. Medford

A quantum Monte Carlo study of the atomization energies for the G2 set of molecules is presented. Basis size dependence of diffusion Monte Carlo atomization energies is studied with a single determinant Slater-Jastrow trial wavefunction…

Chemical Physics · Physics 2015-06-04 F. R. Petruzielo , Julien Toulouse , C. J. Umrigar

The $GW$ approximation has been recently gaining popularity among the method for simulating molecular core-level X-ray photoemission spectra. Traditionally, $GW$ core-level binding energies have been computed using either the cc-pV$n$Z or…

Chemical Physics · Physics 2022-07-13 Daniel Mejia-Rodriguez , Alexander Kunitsa , Edoardo Aprà , Niranjan Govind

We present an application of the blackbox matrix-matrix multiplication (BBMM) algorithm to scale up the Gaussian Process (GP) training of molecular energies in the molecular-orbital based machine learning (MOB-ML) framework. An alternative…

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

Electronic structure calculations, such as in the Hartree-Fock or Kohn-Sham density functional approach, require an initial guess for the molecular orbitals. The quality of the initial guess has a significant impact on the speed of…

Chemical Physics · Physics 2019-03-13 Susi Lehtola

Relativistic quintuple-zeta basis sets for the p elements are presented. The basis sets for the occupied spinors were optimized at the Dirac-Coulomb self-consistent field (SCF) level on the ground configurations. Valence and core…

Over the past six years, molecular transformer models have become key tools in drug discovery. Most existing models are pre-trained on large, unlabeled datasets such as ZINC or ChEMBL. However, the extent to which large-scale pre-training…

Machine Learning · Computer Science 2025-05-23 Afnan Sultan , Max Rausch-Dupont , Shahrukh Khan , Olga Kalinina , Dietrich Klakow , Andrea Volkamer

We propose a novel active learning scheme for automatically sampling a minimum number of uncorrelated configurations for fitting the Gaussian Approximation Potential (GAP). Our active learning scheme consists of an unsupervised machine…

We present a first-principles computer code package (ABACUS) that is based on density functional theory and numerical atomic basis sets. Theoretical foundations and numerical techniques used in the code are described, with focus on the…

Materials Science · Physics 2015-03-03 Pengfei Li , Xiaohui Liu , Mohan Chen , Peize Lin , Xinguo Ren , Lin Lin , Chao Yang , Lixin He

Although quantum computation (QC) is regarded as a promising numerical method for computational quantum chemistry, current applications of quantum-chemistry calculations on quantum computers are limited to small molecules. This limitation…

We introduce property-independent kernels for machine learning modeling of arbitrarily many molecular properties. The kernels encode molecular structures for training sets of varying size, as well as similarity measures sufficiently diffuse…

Chemical Physics · Physics 2015-03-18 Raghunathan Ramakrishnan , O. Anatole von Lilienfeld

Quantum Machine Learning (QML) models of molecular HOMO-LUMO-gaps often struggle to achieve satisfying data-efficiency as measured by decreasing prediction errors for increasing training set sizes. Partitioning training sets of organic…

Chemical Physics · Physics 2021-10-07 Bernard Mazouin , Alexandre Alain Schöpfer , O. Anatole von Lilienfeld
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