Journal
PHYSICAL REVIEW LETTERS
Volume 108, Issue 25, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.108.253005
Keywords
-
Categories
Funding
- Natural Sciences and Engineering Research Council of Canada (NSERC)
- Ontario Graduate Scholarship (OGS) program
Ask authors/readers for more resources
We propose a general method for obtaining accurate valence and Rydberg excitation energies from standard density-functional approximations in adiabatic linear-response time-dependent density-functional theory. The method consists in modeling the sum of Hartree (Coulomb) and exchange-correlation potentials, nu(HXC)(r), by the Hartree-exchange-correlation potential of the corresponding partially ionized system in which a fraction of electron charge (delta = 0.15 to 0.30, depending on the functional) is removed from the highest occupied Kohn-Sham orbital level. The model potential is less repulsive and closer to exact in valence and near asymptotic regions, so it yields more accurate Kohn-Sham orbitals and orbital eigenvalues. By applying this scheme to conventional local, semilocal, and hybrid density-functional approximations, we improve their accuracy for Rydberg excitations by almost an order of magnitude without sacrificing the already good performance for valence transitions.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available