期刊
JOURNAL OF PHYSICAL CHEMISTRY A
卷 115, 期 1, 页码 76-83出版社
AMER CHEMICAL SOC
DOI: 10.1021/jp109280y
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资金
- BYU
- UC Merced
- National Science Foundation [CHE-06-16849-03]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001011]
- UNC EFRC: Solar Fuels and Next Generation Photovoltaics
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [0911119] Funding Source: National Science Foundation
Open-shell singlet diradicals are difficult to model accurately within conventional Kohn-Sham (KS) density-functional theory (DFT). These methods are hampered by spin contamination because the KS determinant wave function is neither a pure spin state nor an eigenfunction of the S-2 operator. Here we present a theoretical foray for using single-reference closed-shell ground states to describe diradicals by fractional-spin DFT (FS-DFT). This approach allows direct, self-consistent calculation of electronic properties using the electron density corresponding to the proper spin eigenfunction. The resulting FS-DFT approach is benchmarked against diradical singlet triplet gaps for atoms and small molecules. We have also applied FS-DFT to the singlet triplet gaps of hydrocarbon polyacenes.
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