Related papers: Saddle Point Search Algorithms for Variational Den…
This paper proposes and analyzes an iterative minimization formulation for search- ing index-1 saddle points of an energy function. This formulation differs from other eigenvector-following methods by constructing a new objective function…
We present a general approach to converge excited state solutions to any quantum chemistry orbital optimization process, without the risk of variational collapse. The resulting Square Gradient Minimization (SGM) approach only requires…
A generalization of the Kohn--Sham approach is derived where the correlation-energy functional depends on the one-particle density matrix of noninteracting states and on the external potential from the interacting target-state. The…
We propose a state-specific orbital optimization scheme for improving the accuracy of excited states of the electronic structure Hamiltonian for the use on near-term quantum computers, which can be combined with any overlap-based…
The most widely-used density functionals for the exchange-correlation energy are inexact for one-electron systems. Their self-interaction errors can be severe in some applications. The problem is not only to correct the self-interaction…
State-specific electronic structure theory provides a route towards balanced excited-state wave functions by exploiting higher-energy stationary points of the electronic energy. Multiconfigurational wave function approximations can describe…
The computational investigation of photochemical processes often entails the calculation of excited state geometries, energies, and energy gradients. The nuclear-electronic orbital (NEO) approach treats specified nuclei, typically protons,…
We present an approach for accurate calculation of exchange energy and total energy for excited states using time independent density functional formalism. This is done by inclusion of gradient correction into the excited state exchange…
Density functional theory (DFT) based modeling of electronic excited states is of importance for investigation of the photophysical/photochemical properties and spectroscopic characterization of large systems. The widely used linear…
A very specific ensemble of ground and excited states is shown to yield an exact formula for any excitation energy as a simple correction to the energy difference between orbitals of the Kohn-Sham ground state. This alternative scheme…
Density functional theory (DFT) is a widespread and effective tool in electronic structure calculations for ground-state electron systems. Its success has prompted exploration into the use of DFT for non-collective excited states. The delta…
Orbit-based methods are widespread in strong-field laser-matter interaction. They provide a framework in which photoelectron momentum distributions can be interpreted as the quantum interference between different semi-classical pathways the…
Kohn-Sham spin-density functional theory provides an efficient and accurate model to study electron-electron interaction effects in quantum dots, but its application to large systems is a challenge. An efficient algorithm for the…
We consider strongly-convex-strongly-concave saddle-point problems with general non-bilinear objective and different condition numbers with respect to the primal and the dual variables. First, we consider such problems with smooth composite…
We extend ground-state density-functional theory to excited states and provide the theoretical formulation for the widely used $\Delta SCF$ method for calculating excited-state energies and densities. As the electron density alone is…
A method for locating first order saddle points on the energy surface of a magnetic system is described and several applications presented where the mechanism of various magnetic transitions is identified. The starting point for the…
Kohn-Sham (KS) density functional theory (DFT) is a very efficient method for calculating various properties of solids as, for instance, the total energy, the electron density, or the electronic band structure. The KS-DFT method leads to…
We consider saddle point problems which objective functions are the average of $n$ strongly convex-concave individual components. Recently, researchers exploit variance reduction methods to solve such problems and achieve linear-convergence…
In the present work, we investigate the computational efficiency afforded by higher-order finite-element discretization of the saddle-point formulation of orbital-free density functional theory. We first investigate the robustness of viable…
The mean-field solutions of electronic excited states are much less accessible than ground state (e.g.\ Hartree-Fock) solutions. Energy-based optimization methods for excited states, like $\Delta$-scf, tend to fall into the lowest solution…