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Orbital-free density functional theory (OF-DFT) provides an alternative approach for calculating the molecular electronic energy, relying solely on the electron density. In OF-DFT, both the ground-state density is optimized variationally to…

Encoding the electronic structure of molecules using 2-electron reduced density matrices (2RDMs) as opposed to many-body wave functions has been a decades-long quest as the 2RDM contains sufficient information to compute the exact molecular…

The Hubbard model provides a test bed to investigate the complex behaviour arising from electron-electron interaction in strongly-correlated systems and naturally emerges as the foundation model for lattice density functional theory (DFT).…

Orbital-free density functional theory (OFDFT) is a quantum chemistry formulation that has a lower cost scaling than the prevailing Kohn-Sham DFT, which is increasingly desired for contemporary molecular research. However, its accuracy is…

Fromager and Lasorne [Electron. Struct. 6 025002 (2024)] have recently derived an in-principle exact Kohn-Sham density functional theory (KS-DFT) of electrons and nuclei, where the nuclear density and the (so-called conditional) electronic…

The universal functional of Hohenberg-Kohn is given as a coupling-constant integral over the density as a functional of the potential. Conditions are derived under which potential-functional approximations are variational. Construction via…

Koopmans spectral functionals are a powerful extension of Kohn-Sham density-functional theory (DFT) that enable the prediction of spectral properties with state-of-the-art accuracy. The success of these functionals relies on capturing the…

The classic density-functional theory (DFT) formalism introduced by Hohenberg, Kohn, and Sham in the mid-1960s, is based upon the idea that the complicated N-electron wavefunction can be replaced with the mathematically simpler 1-electron…

We present an alternative to the Kohn-Sham formulation of density functional theory for the ground-state properties of strongly interacting electronic systems. The idea is to start from the limit of zero kinetic energy and systematically…

Due to its favorable computational efficiency time-dependent (TD) density functional theory (DFT) enables the prediction of electronic spectra in a high-throughput manner across chemical space. Its predictions, however, can be quite…

The formalism of Kohn and Sham uses a specific (model) hamiltonian which highly simplifies the many-electron problem to that of noninteracting fermions. The theorem of Hohenberg and Kohn tells us that, for a given ground state density, this…

The locality hypothesis in density-functional theory (DFT) states that the functional derivative of the Hohenberg-Kohn universal functional can be expressed as a local multiplicative potential function, and this is the basis of DFT and of…

Large scale Density Functional Theory (DFT) based electronic structure calculations are highly time consuming and scale poorly with system size. While semi-empirical approximations to DFT result in a reduction in computational time versus…

The accuracy of density-functional theory (DFT) is determined by the quality of the approximate functionals, such as exchange-correlation in electronic DFT and the excess functional in the classical DFT formalism of fluids. The exact…

The electronic structure calculations based upon energy density functionals are highly successful and widely used both in solid state physics and quantum chemistry. Moreover, the Hohenberg-Kohn theorems and the Kohn-Sham method provide them…

We train a neural network as the universal exchange-correlation functional of density-functional theory that simultaneously reproduces both the exact exchange-correlation energy and potential. This functional is extremely non-local, but…

The treatment of atomic anions with Kohn-Sham density functional theory (DFT) has long been controversial since the highest occupied molecular orbital (HOMO) energy, $E_{HOMO}$, is often calculated to be positive with most approximate…

The exchange-correlation energy in Kohn-Sham density functional theory is expressed as a functional of the electronic density and the Kohn-Sham orbitals. An alternative to Kohn-Sham theory is to express the energy as a functional of the…

Improving the predictive capability of molecular properties in ab initio simulations is essential for advanced material discovery. Despite recent progress making use of machine learning, utilizing deep neural networks to improve quantum…

Variational ab-initio methods in quantum chemistry stand out among other methods in providing direct access to the wave function. This allows in principle straightforward extraction of any other observable of interest, besides the energy,…