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Magnitude and sign of C,C coupling constants in acetylenes and allenes

One‐ and two‐bond C,C coupling constants and the signs of ten of the two‐bond coupling constants were determined from the INADEQUATE and SLAP spectra of four acetylenes and one allene. The geminal C,C coupling constants involving sp‐hybridized carbons are found to be positive and to correlate linearly with the corresponding s character products. In contrast, INDO‐SCPT calculations yield negative values for these coupling constants, and no correlation with the s character products. A separation of those parts of the coupling information transmitted by the σ and π electron framework, based on INDO‐FPT‐PRMO calculations, reveals some possible reasons for the poor performance of the INDO‐SCPT method for systems with π‐electrons.