Related papers: Total energy global optimizations using non orthog…
We introduce an energy functional for ground-state electronic structure calculations. Its variables are the natural spin-orbitals of singlet many-body wave functions and their joint occupation probabilities deriving from controlled…
We derive an automatic procedure for generating a set of highly localized, non-orthogonal orbitals for linear scaling quantum Monte Carlo calculations. We demonstrate the advantage of these orbitals in calculations of the total energy of…
Functionals that strive to correct for such self-interaction errors, such as those obtained by imposing the Perdew-Zunger self-interaction correction or the generalized Koopmans' condition, become orbital dependent or orbital-density…
We demonstrate how to determine numerically nearly exact orthonormal orbitals that are optimal for evaluation of the energy of arbitrary (correlated) states of atoms and molecules by minimization of the energy Lagrangian. Orbitals are…
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…
The current work presents a natural orbital functional (NOF) for electronic systems with any spin value independent of the external potential being considered, that is, a global NOF (GNOF). It is based on a new two-index reconstruction of…
The standard way to calculate the Kohn-Sham orbitals utilizes an approximation of the potential. The approximation consists in a projection of the potential into a finite subspace of basis functions. The orbitals, calculated with the…
In the density functional (DF) theory of Kohn and Sham, the kinetic energy of the ground state of a system of noninteracting electrons in a general external field is calculated using a set of orbitals. Orbital free methods attempt to…
We present a novel route to constructing cost-efficient semi-empirical approximations for the non-additive kinetic energy in subsystem density functional theory. The developed methodology is based on the use of Slater determinants composed…
All-electron calculations play an important role in density functional theory, in which improving computational efficiency is one of the most needed and challenging tasks. In the model formulations, both nonlinear eigenvalue problem and…
We consider a modification of the OMM energy functional which contains an $\ell^1$ penalty term in order to find a sparse representation of the low-lying eigenspace of self-adjoint operators. We analyze the local minima of the modified…
We introduce a novel energy functional for ground-state electronic-structure calculations. Its fundamental variables are the natural spin-orbitals of the implied singlet many-body wave function and their joint occupation probabilities. The…
The choice of molecular orbitals is decisive in configuration interaction calculations. In this letter, a democratic description of the ground and excited states follows an orthogonally constrained orbitals optimization to produce…
Variational quantum eigensolver ans\"atze hold considerable promise for ground-state energy calculations on near-term quantum hardware, yet most promising ansatz designs currently strongly depend on how well the molecular orbital basis…
The implementation of the orbital minimization method (OMM) for solving the self-consistent Kohn-Sham (KS) problem for electronic structure calculations in a basis of non-orthogonal numerical atomic orbitals of finite-range is reported. We…
We present a novel energy-based localization procedure able to localize molecular orbitals into specific spatial regions. The method is applied to several cases including both conjugated and non-conjugated systems. The obtained localized…
We present a method to compute high-order derivatives of the total energy which can be used in the framework of density functional theory. We provide a proof of the $2n+1$ theorem for a general class of energy functionals in which the…
We use the recently introduced single-particle states obtained from localized Deuteron wave-functions as a basis for nuclear many-body calculations. We show that energies can be substantially lowered if the natural orbits obtained from this…
Employing a local formula for the electron-electron interaction energy, we derive a self-consistent approximation for the total energy of a general $N$-electron system. Our scheme works as a local variant of the Thomas-Fermi approximation…
The ground state of atoms from H to Ar was calculated using a self-interaction correction to local and gradient dependent density functionals. The correction can significantly improve the total energy and makes the orbital energies…