Abstract
Ab initio calculations are reported for the isotropic hyperfine coupling constants for sigma (vinyl and ethynyl) and nonconjugated pi (methyl) radicals using the unrestricted, projected, and extended Hartree–Fock methods. It is found that quartet state annihilation procedures closely approximate the results obtained by full projection of the UHF wave function using an STO‐3G basis set. The extended Hartree–Fock method is discussed to explain why it overestimates the spin polarization mechanism. Possible alternatives to the UHF method are discussed.

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