Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 136, Issue 12, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/1.3696967
Keywords
ab initio calculations; density functional theory; excited states; orbital calculations; SCF calculations; variational techniques
Funding
- NSERC
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We present here the implementation of a self-consistent approach to the calculation of excitation energies within regular Kohn-Sham density functional theory. The method is based on the n-order constricted variational density functional theory (CV(n)-DFT) [T. Ziegler, M. Seth, M. Krykunov, J. Autschbach, and F. Wang, J. Chem. Phys. 130, 154102 (2009)] and its self-consistent formulation (SCF-CV(infinity)-DFT) [J. Cullen, M. Krykunov, and T. Ziegler, Chem. Phys. 391, 11 (2011)]. A full account is given of the way in which SCF-CV(infinity)-DFT is implemented. The SCF-CV(infinity)-DFT scheme is further applied to transitions from occupied pi orbitals to virtual pi* orbitals. The same series of transitions has been studied previously by high-level ab initio methods. We compare here the performance of SCF-CV(infinity)-DFT to that of time dependent density functional theory (TD-DFT), CV(n)-DFT and Delta SCF-DFT, with the ab initio results as a benchmark standard. It is finally demonstrated how adiabatic TD-DFT and Delta SCF-DFT are related through different approximations to SCF-CV(infinity)-DFT. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.3696967]
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