arXiv subjects

Dahvyd Wing

Publications and source records attributed to Dahvyd Wing.

5 recordsLinked to original sources

arXiv2026

Accurate and Transferable Intermolecular Potential Based on Machine-Learned Molecular Electron Density

Machine-learned force fields (MLFFs) contain many learnable parameters and therefore require large training datasets. This poses a challenge for developing highly accurate, general-purpose MLFFs because generating high-quality ab initio reference data is computationally expensive. Classical empirical potentials offer a potentially inexpensive source of synthetic training data, but existing models often lack the accuracy needed to provide useful reference energies. Here, we introduce the density-based intermolecular potential (DensIP), a physics-based model of intermolecular interactions that uses machine-learned electron densities and only four universal parameters. We train and test DensIP on CCSD(T)/CBS interaction energies from DES15K, a dataset of dimers of small organic molecules. DensIP achieves sub-kcal/mol errors for dimers containing molecules absent from the training set, including molecules in non-equilibrium conformations, demonstrating strong transferability. We further show that DensIP can be applied to molecules as large as drug ligands. Notably, DensIP outperforms state-of-the-art general-purpose MLFFs for long-range interactions, making it a promising approach for generating accurate synthetic training data at scale.

physics.chem-ph↗

arXiv2025

A Transferable Model of Molecular Exchange-Repulsion Interaction from Anisotropic Valence Density Overlap

Pauli exchange-repulsion is the dominant short-range intermolecular interaction and it is an essential component of molecular force fields. Current approaches to modeling Pauli repulsion in molecular force fields often rely on over 20 atom types to achieve chemical accuracy, illustrating the challenge in finding models which have broadly transferable parameters, which hampers the development of force fields with quantum-chemical accuracy that are transferable across many chemical systems. We present the anisotropic valence density overlap (AVDO) model for exchange-repulsion. The model produces sub-kcal/mol accuracy for dimers of organic molecules and contains two universal parameters, which we demonstrate are transferable for molecules composed of H, C, N, O, F, P, S, Cl, and Br. The model is tested on 1,872 unique molecular pairs selected from a set of 135 molecules, and samples dissociation curves and configurations from condensed-phase molecular dynamics trajectories. Given recent progress in machine learning of the electronic density, this model offers a promising path toward high-accuracy, next-generation machine-learned force fields.

physics.chem-ph↗

arXiv2023

Optical absorption spectra of metal oxides from time-dependent density functional theory and many-body perturbation theory based on optimally-tuned hybrid functionals

Using both time-dependent density functional theory (TDDFT) and the ``single-shot" $GW$ plus Bethe-Salpeter equation ($GW$-BSE) approach, we compute optical band gaps and optical absorption spectra from first principles for eight common binary and ternary closed-shell metal oxides (MgO, Al$_2$O$_3$, CaO, TiO$_2$, Cu$_2$O, ZnO, BaSnO$_3$, and BiVO$_4$), based on the non-empirical Wannier-localized optimally-tuned screened range-separated hybrid functional. Overall, we find excellent agreement between our TDDFT and $GW$-BSE results and experiment, with a mean absolute error less than 0.4 eV, including for Cu$_2$O and ZnO, traditionally considered to be challenging for both methods.

cond-mat.mtrl-sci↗

arXiv2022

An Optimally-Tuned Starting Point for Single-Shot $GW$ Calculations of Solids

The dependence of ab initio many-body perturbation theory within the $GW$ approximation on the eigensystem used in calculating quasiparticle corrections limits this method's predictive power. Here, we investigate the accuracy of the recently developed Wannier-localized optimally tuned screened range-separated hybrid (WOT-SRSH) functional as a generalized Kohn-Sham starting point for single-shot $GW$ ($G_0W_0$) calculations for a range of semiconductors and insulators. Comparison to calculations based on well-established functionals, namely PBE, PBE0, and HSE, as well as to self-consistent $GW$ schemes and to experiment, shows that band gaps computed via $G_0W_0$@WOT-SRSH have a level of precision and accuracy that is comparable to that of more advanced methods such as quasiparticle self-consistent $GW$ (QS$GW$) and eigenvalue self-consistent $GW$ (ev$GW$). We also find that $G_0W_0$@WOT-SRSH improves the description of states deeper in the valence band manifold. Finally, we show that $G_0W_0$@WOT-SRSH significantly reduces the sensitivity of computed band gaps to ambiguities in the underlying WOT-SRSH tuning procedure.

cond-mat.mtrl-sci↗

arXiv2021

Band gaps of crystalline solids from Wannier-localization based optimal tuning of a screened range-separated hybrid functional

Accurate prediction of fundamental band gaps of crystalline solid state systems entirely within density functional theory is a long standing challenge. Here, we present a simple and inexpensive method that achieves this by means of non-empirical optimal tuning of the parameters of a screened range-separated hybrid functional. The tuning involves the enforcement of an ansatz that generalizes the ionization potential theorem to the removal of an electron in an occupied state described by a localized Wannier function in a modestly sized supercell calculation. The method is benchmarked against experiment for a set of systems ranging from narrow band gap semiconductors to large band gap insulators, spanning a range of fundamental band gaps from 0.2 to 14.2 eV and is found to yield quantitative accuracy across the board, with a mean absolute error of $\sim$0.1 eV and a maximal error of $\sim$0.2 eV.

cond-mat.mtrl-sci↗