相关论文: A generalized exchange-correlation functional: the…

In a previous contribution (Mol. Phys. {\bf 103}, xxxx, 2005), we established the suitability of density functional theory (DFT) for the calculation of molecular anharmonic force fields. In the present work, we have assessed a wide variety…

The balance between localised and delocalised electron distribution in the N,N'-dimethylpiperazine (DMP) molecule in the 3s Rydberg excited state and in the fully ionised DMP$^+$ provides a valuable test of density functionals, in…

It is shown that the DFT exchange and correlation functionals satisfy an expression that couples exchange and correlation functionals and functional derivatives evaluated at three different densities and for two particle numbers. This…

We present the WCCR10 data set of ten ligand dissociation energies of large cationic transition metal complexes for the assessment of approximate exchange--correlation functionals. We analyze nine popular functionals, namely BP86, BP86-D3,…

Embedded density functional theory (e-DFT) is used to describe the electronic structure of strongly interacting molecular subsystems. We present a general implementation of the Exact Embedding (EE) method [J. Chem. Phys. 133, 084103 (2010)]…

Deorbitalization of a conventional meta-generalized-gradient exchange-correlation approximation replaces its dependence upon the Kohn-Sham kinetic energy density with a dependence on the density gradient and Laplacian. In principle, that…

We present and discuss some ideas concerning an ``average-pair-density functional theory'', in which the ground-state energy of a many-electron system is rewritten as a functional of the spherically and system-averaged pair density. These…

Machine-learned potentials (MLPs) have become a popular approach of modelling interatomic interactions in atomistic simulations, but to keep the computational cost under control, a relatively short cutoff must be imposed, which put serious…

Density functional theory (DFT) is probably the most promising approach for quantum chemistry calculations considering its good balance between calculations precision and speed. In recent years, several neural network-based functionals have…

This work presents a new class of hybrid density functional theory (DFT) approximations, incorporating nonlocal exact exchange in predefined states such as core atomic orbitals (AOs). These projected hybrid density functionals are a…

The construction of density-functional approximations is explored by modeling the adiabatic connection em locally, using energy densities defined in terms of the electrostatic potential of the exchange-correlation hole. These local models…

Understanding and controlling the informational complexity of neural networks is a central challenge in machine learning, with implications for generalization, optimization, and model capacity. While most approaches rely on entropy-based…

Hydrogen bonding is an important non-covalent interaction that plays a major role in molecular self-organization and supramolecular structures. It can be described accurately with ab initio quantum chemical wave function methods, which…

Neural networks are being used to make new types of empirical chemical models as inexpensive as force fields, but with accuracy close to the ab-initio methods used to build them. Besides modeling potential energy surfaces, neural-nets can…

We develop a modified Poisson-Nernst-Planck model which includes both the long-range Coulomb and short-range hard-sphere correlations in its free energy functional such that the model can accurately describe the ion transport in complex…

We present here novel insight into exchange-correlation functionals in density functional theory, based on the viewpoint of optimal transport. We show that in the case of two electrons and in the semiclassical limit, the exact…

We performed a benchmark study on a series of dihydrogen bond complexes and constructed a set of reference bond distances and interaction energies. The test set was employed to assess the performance of several wave-function correlated and…

One of the central challenges in modern machine learning is understanding how neural networks generalize knowledge learned from training data to unseen test data. While numerous empirical techniques have been proposed to improve…

It seems self-evident that a density functional calculation should be normalized to the number of electrons in the system. We present multiple examples where the accuracy of the approximate energy is improved (sometimes greatly) by…

A geometry-based density functional theory is presented for mixtures of hard spheres, hard needles and hard platelets; both the needles and the platelets are taken to be of vanishing thickness. Geometrical weight functions that are…