Related papers: Non-Adiabatic Approximations in Time-Dependent Den…
Ensemble density functional theory (eDFT) is an exact time-independent alternative to time-dependent DFT (TD-DFT) for the calculation of excitation energies. Despite its formal simplicity and advantages in contrast to TD-DFT (multiple…
Time-dependent density-functional theory (TDDFT) is a formally exact approach to the time-dependent electronic many-body problem which is widely used for calculating excitation energies. We present a survey of the fundamental framework,…
We show that as an electron transfers between closed-shell molecular fragments at large separation, the exact correlation potential of time-dependent density functional theory gradually develops a step and peak structure in the bonding…
The adiabatic approximation in time-dependent density functional theory (TDDFT) is known to give an incorrect pole structure in the quadratic response function, leading to unphysical divergences in excited state-to-state transition…
The Kohn-Sham approach to time-dependent density-functional theory (TDDFT) can be formulated, in principle exactly, by invoking the force-balance equation for the density, which leads to an explicit expression for the exchange-correlation…
We perform model calculations for a stretched LiF molecule, demonstrating that nonadiabatic charge transfer effects can be accurately and seamlessly described within a density functional framework. In alkali halides like LiF, there is an…
The role of the exchange-correlation potential and the exchange-correlation kernel in the calculation of excitation energues from time-dependent density functional theory is studied. Excitation energies of the He and Be atoms are…
An adiabatic-connection fluctuation-dissipation theorem approach based on a range separation of electron-electron interactions is proposed. It involves a rigorous combination of short-range density functional and long-range random phase…
In order to assess the accuracy of commonly used approximate exchange-correlation density functionals, we present a comparison of accurate exchange and correlation potentials, exchange energy densities and energy components with the…
Interpolating the exchange-correlation energy along the density-fixed adiabatic connection of density functional theory is a promising way to build approximations that are not biased towards the weakly correlated regime. These…
Rabi oscillations have long been thought to be out of reach in simulations using time-dependent density functional theory (TDDFT), a prominent symptom of the failure of the adiabatic approximation for non-perturbative dynamics. We present a…
The possibility of finding multistability in the density and current of an interacting nanoscale junction coupled to semi-infinite leads is studied at various levels of approximation. The system is driven out of equilibrium by an external…
We study non-linear adiabatic connection paths in density-functional theory using modified electron-electron interactions that perform a long-range/short-range separation of the Coulomb interaction. These adiabatic connections allows to…
We consider the electrons of a molecule in the adiabatic time-dependent density functional theory approximation. We establish the well-posedness of the time evolution and its linear response close to a non-degenerate ground state, and prove…
We formulate a rigorous method for calculating a nonadiabatic (frequency-dependent) exchange-correlation (XC) kernel required for correct description of both equilibrium and nonequilibrium properties of strongly correlated systems within…
Time-dependent density-functional theory (TDDFT) is a powerful tool to study the non-equilibrium dynamics of inhomogeneous interacting many-body systems. Here we show that the simple adiabatic local-spin-density approximation for the…
Density functional theory at finite temperatures often relies on the zero-temperature approximation, which uses a ground-state exchange-correlation functional with thermalized densities. This approach, however, neglects the explicit…
We derive a time-dependent density functional theory appropriate for calculating the near-edge X-ray absorption spectrum in molecules and condensed matter. The basic assumption is to increase the space of many-body wave functions from one…
An approximate solution to the time-dependent density functional theory (TDDFT) response equations for finite systems is developed, yielding corrections to the single-pole approximation. These explain why allowed Kohn-Sham transition…
There is currently much interest in the development of improved trajectory-based methods for the simulation of nonadiabatic processes in complex systems. An important goal for such methods is the accurate calculation of the rate constant…