相关论文: Delta Self-Consistent Field as a method to obtain …

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…

Accurate and efficient simulation of excited state properties is an important and much aspired cornerstone in the study of adsorbate dynamics on metal surfaces. To this end, the recently proposed linear expansion \Delta Self-Consistent…

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…

Delta-self-consistent field theory (delta-SCF) is a conceptually simple and computationally inexpensive method for finding excited states. Using the maximum overlap method to guide optimization of the excited state, delta-SCF has been shown…

This chapter provides a basic introduction to excited-state extensions of density functional theory (DFT), including time-dependent (TD-)DFT in both its linear-response and its explicitly time-dependent formulations. As applied to the…

This chapter presents the development of a density functional theory (DFT)-based method for accurate, reliable treatment of various resonances in atoms. Many of these are known to be notorious for their strong correlation, proximity to more…

We present a first principles strategy for developing state-specific density functional approximations for excited states. We first clarify why approaches based on conventional ground state approximations miss density-driven correlations,…

Spectroscopies that probe electronic excitations from core levels into unoccupied orbitals, such as X-ray absorption spectroscopy and electron energy loss spectroscopy, are widely used to gain insight into the electronic and chemical…

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…

For the computational prediction of core electron binding energies in solids, two distinct kinds of modelling strategies have been pursued: the $\Delta$-Self-Consistent-Field method based on density functional theory (DFT), and the GW…

Variational excited-state density functional theory (DFT) enables the calculation of excited states at a cost comparable to ground-state calculations, but single-configuration approaches often suffer from spin contamination. We implement…

A direct orbital optimization method is presented for density functional calculations of excited electronic states using either a real space grid or a plane wave basis set. The method is variational, provides atomic forces in the excited…

Use of density-functional theory in a $\Delta$self-consistent field framework result in both the ground- and two lowest electronicly excited states of the NaCl and LiCl. The accuracy of this method is confirmed using a multi-configuration…

We prove the general chemical potential theorem: the noninteracting one-electron orbital energies in DFT ground states and $\Delta$SCF excited states are corresponding chemical potentials of electron addition or removal, from an…

The implementation of an efficient self-consistent field (SCF) method including both scalar relativistic effects and spin-orbit interaction in density functional theory (DFT) is presented. We make use of Gaussian-type orbitals (GTOs) and…

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…

Density functional theory (DFT) and beyond-DFT methods are often used in combination with photoelectron spectroscopy to obtain physical insights into the electronic structure of molecules and solids. The Kohn-Sham eigenvalues are not…

Typical density functional theory (DFT) and approximations thereto solve the many-electron ground state problem by working from a numerically efficient non-interacting Kohn-Sham reference system; and benefit from useful minimization…

To describe excited states, the electron density alone being insufficient, we use the noninteracting reference density matrix $\gamma_{s}({\bf x},{\bf x}')$ based on the recently established foundation for the $\Delta SCF$ theory, in which…

Despite the variety of available computational approaches, state-of-the-art methods for calculating excitation energies such as time-dependent density functional theory (TDDFT), are computationally demanding and thus limited to moderate…