Related papers: Eliminating Delocalization Error through Localized…

Localized molecular orbitals are often used for the analysis of chemical bonds, but they can also serve to efficiently and comprehensibly compute linear response properties. While conventional canonical molecular orbitals provide an…

This paper proposes an enhanced list-aided successive cancellation stack (ELSCS) decoding algorithm with adjustable decoding complexity. In addition, a logarithmic likelihood ratio (LLR)-threshold based path extension scheme is designed to…

We study static correlation and delocalisation errors and show that even methods with good energies can yield significant delocalization errors that affect the density, leading to large errors in predicting {\em e.g.} dipole moments. We…

We present a fully variational locally scaled self-interaction corrected (SIC) energy functional using complex optimal orbitals. This represents an important milestone for fully variational SIC energy functionals, which have been shown to…

We present for the first time an efficient iterative method to directly solve the four-component Dirac-Kohn-Sham (DKS) density functional theory. Due to the existence of the negative energy continuum in the DKS operator, the existing…

The band-gap problem and other systematic failures of approximate functionals are explained from an analysis of total energy for fractional charges. The deviation from the correct intrinsic linear behavior in finite systems leads to…

Quasiparticle energies and fundamental band gaps in particular are critical properties of molecules and materials. It was rigorously established that the generalized Kohn-Sham HOMO and LUMO orbital energies are the chemical potentials of…

A detailed account of the implementation of equations of the Relativistic Density Functional Theory (RDFT) using basis sets of APW/LAPW type with flexible extensions provided by local orbitals is given. Earlier discoveries of the importance…

Delocalization errors, such as charge-transfer and some self-interaction errors, plague computationally-efficient and otherwise-accurate density functional approximations (DFAs). Evaluating a semi-local DFA non-self-consistently on the…

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…

Background: An electron localization function was originally introduced to visualize bond structures in molecules. It became a useful tool to describe electron configurations in atoms, molecules and solids. In nuclear physics, a nucleon…

This chapter presents controlled approximations of Kohn-Sham density functional theory (DFT) that enable very large scale simulations. The work is motivated by the study of defects in crystalline solids, though the ideas can be used in…

DFT calculations have become widespread in both chemistry and materials, because they usually provide useful accuracy at much lower computational cost than wavefunction-based methods. All practical DFT calculations require an approximation…

We propose a method to probe the local density of states (LDOS) of atomic systems that provides both spatial and energy resolution. The method combines atomic and tunneling techniques to supply a simple, yet quantitative and operational,…

A new method for calculating optical absorption spectra within linear-scaling density-functional theory (LS-DFT) is presented, incorporating a scheme for optimizing a set of localized orbitals to accurately represent unoccupied Kohn-Sham…

We propose a novel scheme to bring reduced density matrix functional theory (RDMFT) into the realm of density functional theory (DFT) that preserves the accurate density functional description at equilibrium, while incorporating accurately…

Current quantization methods for LLMs predominantly rely on block-wise structures to maintain efficiency, often at the cost of representational flexibility. In this work, we demonstrate that element-wise quantization can be made as…

Density-functional theory (DFT) has revolutionized computer simulations in chemistry and material science. A faithful implementation of the theory requires self-consistent calculations. However, this effort involves repeatedly diagonalizing…

Locality of compact one-electron orbitals expanded strictly in terms of local subsets of basis functions can be exploited in density functional theory (DFT) to achieve linear growth of computation time with systems size, crucial in…

Given a set of Kohn-Sham orbitals from an insulating system, we present a simple, robust, efficient and highly parallelizable method to construct a set of, optionally orthogonal, localized basis functions for the associated subspace. Our…