Related papers: Charge-constrained Atomic Cluster Expansion
Modeling distributions of covariates, or density estimation, is a core challenge in unsupervised learning. However, the majority of work only considers the joint distribution, which has limited utility in practical situations. A more…
We present a method to constrain local charge multipoles within density-functional theory. Such multipoles quantify the anisotropy of the local charge distribution around atomic sites and can indicate potential hidden orders. Our method…
Cluster expansion (CE) is effective in modeling the stability of metallic alloys, but sometimes cluster expansions fail. Failures are often attributed to atomic relaxation in the DFT-calculated data, but there is no metric for quantifying…
Static correlation error(SCE) inevitably emerges when a dissociation of a covalent bond is described with a conventional denstiy-functional theory (DFT) for electrons. SCE gives rise to a serious overshoot in the potential energy at the…
We present a computational scheme for extracting the energy level alignment of a metal/molecule interface, based on constrained density functional theory and local exchange and correlation functionals. The method, applied here to benzene on…
A new reference state for density functional theory, termed the independent atom ansatz, is introduced in this work. This ansatz allows for the exact representation of electron density in terms of non-interacting, atom-localized orbitals.…
The framework of nuclear energy density functionals is applied to a study of the formation and evolution of cluster states in nuclei. The relativistic functional DD-ME2 is used in triaxial and reflection-asymmetric relativistic…
The present study aims at further development of covariant energy density functionals (CEDFs) towards more accurate description of binding energies across the nuclear chart. For the first time, infinite basis corrections to binding energies…
Linear scaling density functional theory approaches to electronic structure are often based on the tendency of electrons to localize even in large atomic and molecular systems. However, in many cases of actual interest, for example in…
The charge delocalization error, besides nondynamic correlation, has been a major challenge to density functional theory. Contemporary functionals undershoot the dissociation of symmetric charged dimers A2+, a simple but stringent test,…
Constrained density functional theory (cDFT) is a versatile electronic structure method that enables ground-state calculations to be performed subject to physical constraints. It thereby broadens their applicability and utility. Automated…
Accurately modeling chemical reactions at the atomistic level requires high-level electronic structure theory due to the presence of unpaired electrons and the need to properly describe bond breaking and making energetics. Commonly used…
We investigate the formation of polycrystalline structures in a class of particle systems. The atomistic energy is modeled as a sum of particle energies that favor atoms being locally isometric to a reference lattice. The discrete frame…
Non-adiabatic effects play an important role in many chemical processes. In order to study the underlying non-adiabatic potential-energy surfaces (PESs), we present a locally-constrained density-functional theory approach, which enables us…
The silicon-hydrogen system is of key interest for solar-cell devices, including both crystalline and amorphous modifications. Elemental amorphous Si is now well understood, but the atomic-scale effects of hydrogenating the silicon matrix…
Methods for estimating the correlation energy of molecules and other electronic systems are discussed based on the assumption that the correlation energy can be partitioned between atomic regions. In one method, the electron density is…
An in-principle exact working equation to compute electronic affinity and ionization Fukui functions is derived within the $N$-centered (Nc) ensemble extension of density functional theory (DFT). It circumvents the kernel derivative…
Charged excitations are electronic transitions that involve a change in the total charge of a molecule or material. Understanding the properties and reactivity of charged species requires insights from theoretical calculations that can…
We propose a simple scheme to construct composition-dependent interatomic potentials for multicomponent systems that when superposed onto the potentials for the pure elements can reproduce not only the heat of mixing of the solid solution…
Approximate functionals used in practical density functional theory (DFT) deviate from the piecewise linear behavior of the exact functional for fractional charges. This deviation causes excess charge delocalization, which leads to…