相关论文: Response calculations based on an independent part…
The many-body $GW$ formalism, for the calculation of ionization potentials or electronic affinities, relies on the frequency-dependent dielectric function built from the electronic degrees of freedom. Considering the case of water as a…
Static electric response properties of atoms and molecules are reported within the real-space Cartesian grid implementation of pseudopotential Kohn-Sham (KS) density functional theory (DFT). A detailed systematic investigation is made for a…
A new reference state for density functional theory, termed the independent atom ansatz, is introduced in this work. This ansatz allows for the exact representation of electron density in terms of non-interacting, atom-localized orbitals.…
The static second hyperpolarizability is derived from the space-fractional Schr\"{o}dinger equation in the particle-centric view. The Thomas-Reiche-Kuhn sum rule matrix elements and the three-level ansatz determines the maximum second…
By introducing the self-energy density functionals for the dissipative interactions between the reduced system and its environment, we develop a time-dependent density-functional theory formalism based on an equation of motion for the…
The accurate prediction of electronic response properties of extended molecular systems has been a challenge for conventional, explicit density functionals. We demonstrate that a self-interaction correction implemented rigorously within…
Response calculations in density functional theory aim at computing the change in ground-state density induced by an external perturbation. At finite temperature these are usually performed by computing variations of orbitals, which involve…
A frequency-dependent extension of the polarizable force field ``Atom-Condensed Kohn-Sham density functional theory approximated to the second-order'' (ACKS2) [J. Chem. Phys. 141, 194114 (2014)] is proposed, referred to as ACKS2$\omega$.…
We present a new time-dependent Density Functional approach to study the relaxational dynamics of an assembly of interacting particles subject to thermal noise. Starting from the Langevin stochastic equations of motion for the velocities of…
We show that the time dependent single electron, nuclear density matrix of an interacting electronic system coupled to nuclear degrees of freedom can be exactly reproduced by that of an electronic system with arbitrarily specified…
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 formulate a hyperspherical approach within standard configuration interaction calculations aiming at a description of large-scale dynamics of $N$-particle system. The channel wave function and the adiabatic channel energy are determined…
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…
Polarizability is a key response property of physical and chemical systems, which has an impact on intermolecular interactions, spectroscopic observables, and vacuum polarization. The calculation of polarizability for quantum systems…
We show that electrodynamic dipolar interactions, responsible for long-range fluctuations in matter, play a significant role in the stability of molecular crystals. Density functional theory calculations with van der Waals interactions…
Previous studies have used numerical methods to optimize the hyperpolarizability of a one-dimensional quantum system. These studies were used to suggest properties of one-dimensional organic molecules, such as the degree of modulation of…
The dynamic atomic polarizability describes the response of the atom to incoming electromagnetic radiation. The functional form of the imaginary part of the polarizability for small driving frequencies omega has been a matter of…
The reliability of the approximations commonly adopted in the calculation of static optical (hyper)polarizabilities is tested against exact results obtained for an interesting toy-model. The model accounts for the principal features of…
In the current density functional theory of linear and nonlinear time-dependent phenomena, the treatment of exchange and correlation beyond the level of the adiabatic local density approximation is shown to lead to the appearance of…
A new numerical method is proposed for determining the low-frequency dynamics of the charge carrier coupled to the deformable quantum lattice. As an example, the polaron band structure is calculated for the one-dimensional Holstein model.…