Assessment of the ΔSCF-DFT approach for electronic excitations in organic dyes
Author(s)Kowalczyk, Timothy Daniel; Yost, Shane Robert; Van Voorhis, Troy
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This paper assesses the accuracy of the ΔSCF method for computing low-lying HOMO→LUMO transitions in organic dye molecules. For a test set of vertical excitation energies of 16 chromophores, surprisingly similar accuracy is observed for time-dependent density functional theory and for ΔSCF density functional theory. In light of this performance, we reconsider the ad hoc ΔSCF prescription and demonstrate that it formally obtains the exact stationary density within the adiabatic approximation, partially justifying its use. The relative merits and future prospects of ΔSCF for simulating individual excited states are discussed.
DepartmentMassachusetts Institute of Technology. Department of Chemistry
Journal of Chemical Physics
American Institute of Physics
Kowalczyk, Tim, Shane R. Yost, and Troy Van Voorhis. “Assessment of the ΔSCF Density Functional Theory Approach for Electronic Excitations in Organic Dyes.” The Journal of Chemical Physics 134.5 (2011): 054128. Web.
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