Journal
PHYSICAL REVIEW B
Volume 86, Issue 20, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevB.86.205110
Keywords
-
Funding
- NSF CRIF [CHE-0946869]
- Georgia Institute of Technology
- AFOSR through the COMAS MURI [FA9550-10-1-0558]
- AvH Foundation
- US Department of Energy [DE-FG02-97ER25308]
- US National Science Foundation [CHE-1011360]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1011360] Funding Source: National Science Foundation
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [0946869] Funding Source: National Science Foundation
Ask authors/readers for more resources
Long-range corrected hybrid functionals that employ a nonempirically tuned range-separation parameter have been demonstrated to yield accurate ionization potentials and fundamental gaps for a wide range of finite systems. Here, we address the question of whether this high level of accuracy is limited to the highest occupied/lowest unoccupied energy levels to which the range-separation parameter is tuned or whether it is retained for the entire valence spectrum. We examine several pi-conjugated molecules and find that orbitals of a different character and symmetry require significantly different range-separation parameters and fractions of exact exchange. This imbalanced treatment of orbitals of a different nature biases the resulting eigenvalue spectra. Thus, the existing schemes for the tuning of range-separated hybrid functionals, while providing for good agreement between the highest occupied energy level and the first ionization potential, do not achieve accuracy comparable to reliable G(0)W(0) computations for the entire quasiparticle spectrum.
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