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The accurate calculation of electronic potential energy surfaces for ground and excited states is crucial for understanding photochemical processes, particularly near conical intersections. While classical methods are limited by scaling and…
The analytic energy gradients with respect to nuclear motion are derived for natural orbital functional (NOF) theory. The resulting equations do not require to resort to linear-response theory, so the computation of NOF energy gradients is…
For orbital-free {\it ab initio} molecular dynamics, especially on systems in extreme thermodynamic conditions, we provide the first pseudo-potential-adapted generalized gradient approximation (GGA) functional for the non-interacting free…
An efficient computational algorithm to implement a local operator approach to partitioning electronic energy in general molecular systems is presented. This approach, which rigorously defines the electronic energy on any subsystem within a…
We introduce an orbital free electron density functional approximation based on alchemical perturbation theory. Given convergent perturbations of a suitable reference system, the accuracy of popular self-consistent Kohn-Sham density…
A method for increasing the accuracy of configuration interaction (CI) calculations of molecules and other electronic systems is proposed. The energy defect of a given calculation is associated with the electron pair origin of…
The piecewise linearity condition on the total energy with respect to the total magnetization of finite quantum systems is derived, using the infinite-separation-limit technique. This generalizes the well-known constancy condition, related…
By using results of highly accurate computations of the total energies of a large number of few-electron atoms we construct a few interpolation formulas which can be used to approximate the total energies of bound atomic states. In our…
This work assesses the performance of the recently proposed global natural orbital functional (GNOF) against the charge delocalization error. GNOF provides a good balance between static and dynamic electronic correlation leading to accurate…
A novel energy minimization formulation of electrostatics that allows computation of the electrostatic energy and forces to any desired accuracy in a system with arbitrary dielectric properties is presented. An integral equation for the…
Orbital-free density functional theory (OFDFT) offers a challenging way of electronic-structure calculations scaled as $\mathcal{O}(N)$ computation for system size $N$. We here develop a scheme of the OFDFT calculations based on the…
We demonstrate that Daubechies wavelets can be used to construct a minimal set of optimized localized contracted basis functions in which the Kohn-Sham orbitals can be represented with an arbitrarily high, controllable precision. Ground…
We provide several quantum algorithms for continuous optimization that do not require gradient estimation. Instead, we encode the optimization problem into the dynamics of a physical system and coherently simulate the time evolution. We…
A widely used strategy to reduce the computational cost in quantum-chemical calculations is to partition the system into an active subsystem, which is the focus of the computational efforts and an environment that is treated at a lower…
Computing many-body ground state energies and resolving electronic structure calculations are fundamental problems for fields such as quantum chemistry or condensed matter. Several quantum computing algorithms that address these problems…
An analysis of orbital magnetization in band insulators is provided. It is shown that a previously proposed electronic orbital angular-momentum operator generalizes the ``modern theory of orbital magnetization'' to include non-local…
Localized basis sets in the projector augmented wave formalism allow for computationally efficient calculations within density functional theory (DFT). However, achieving high numerical accuracy requires an extensive basis set, which also…
Within the framework of linear-scaling Kohn-Sham density functional theory, a robust method for maintaining compact localized orbitals close to the ground state is coupled with nuclear dynamics. This allows to obviate the commonly employed…
For the classical N-body problem, an approach is proposed based on the introduction of some natural in the physical sense optimization problems of mathematical programming for finding a conditional minimum for the characteristics of the…
In the past decade, natural orbital functional (NOF) approximations have emerged as prominent tools for characterizing electron correlation. Despite their effectiveness, these approaches, which rely on natural orbitals and their associated…