Benchmarking Functionals for Strong-Field Light-Matter Interactions in Adiabatic Time-Dependent Density Functional Theory.

In recent years, time-dependent density functional theory (TDDFT) has been extensively employed for highly nonlinear optics in molecules and solids, including high harmonic generation (HHG), photoemission, and more. TDDFT exhibits a relatively low numerical cost while still describing both light-matter and electron-electron interactions ab initio, making it highly appealing. However, the majority of implementations of the theory utilize the simplest possible approximations for the exchange-correlation (XC) functional-either the local density or generalized gradient approximations, which are traditionally considered to have rather poor chemical accuracy.

Exchange-only virial relation from the adiabatic connection.

The exchange-only virial relation due to Levy and Perdew is revisited. Invoking the adiabatic connection, we introduce the exchange energy in terms of the right-derivative of the universal density functional w.r.

Exchange energies with forces in density-functional theory.

We propose exchanging the energy functionals in ground-state density-functional theory with physically equivalent exact force expressions as a new promising route toward approximations to the exchange-correlation potential and energy. In analogy to the usual energy-based procedure, we split the force difference between the interacting and auxiliary Kohn-Sham system into a Hartree, an exchange, and a correlation force. The corresponding scalar potential is obtained by solving a Poisson equation, while an additional transverse part of the force yields a vector potential.

Self-interaction correction schemes for non-collinear spin-density-functional theory.

We extend some of the well-established self-interaction correction (SIC) schemes of density-functional theory-the Perdew-Zunger SIC and the average-density SIC-to the case of systems with noncollinear magnetism. Our proposed SIC schemes are tested on a set of molecules and metallic clusters in combination with the widely used local spin-density approximation. As expected from the collinear SIC, we show that the averaged-density SIC works well for improving ionization energies but fails to improve more subtle quantities like the dipole moments of polar molecules.