The infrared spectra (3500 to 40 cm Γ1 ) of gaseous and solid and the Raman spectra (3500 to 30 cm Γ1 ) of liquid and solid 1-fluorosilacyclobutane, c-C 3 H 6 SiFH, have been obtained. Both the axial and equatorial conformers with respect to the fluorine atom have been identified in the fluid phases. Variable temperature (Γ105 to Γ150 Β°C) studies of the infrared spectra of the sample dissolved in liquid krypton have been carried out. From these data, the enthalpy difference has been determined to be 282 Β± 27 cm Γ1 (3.37 Β± 0.32 kJ/ mol), with the equatorial conformer the more stable form and the only conformer remaining in the annealed solid. At ambient temperature there is approximately 21 Β± 2% of the axial conformer present in the vapor phase. From isolated Si-H stretching frequencies the Si-H (r 0 ) distances are calculated to be 1.484 and 1.485 A Λfor the equatorial and axial conformers, respectively. Structural parameters have been predicted from MP2/6-311 + G(d,p) ab initio calculations and the adjusted r 0 parameters for both conformers were obtained from a combination of the ab initio predicted values and the six previously reported microwave rotational constants. Along with the Si-H bond distance, the Si-C, and C-C distances of 1.865(5), and 1.571(5) A Λ, respectively, for the equatorial conformer are significantly different from the values for these parameters previously reported from an election diffraction study. Both the SiC and CC distances and the SiF distance are longer by 0.002 and 0.004 A Λ, respectively, for the axial conformer. Structural parameters have also been obtained for silacyclobutane, c-C 3 H 6 SiH 2 and ethylsilylfluoride, CH 3 CH 2 SiH 2 F, from combined ab initio predicted values and previously reported rotational constants. Several of these newly determined parameters are significantly different from those previously reported for both molecules. Complete equilibrium geometries, conformational stabilities, harmonic force fields, infrared intensities, Raman activities, and depolarization ratios have been determined for both rotamers by ab initio calculations employing the 6-31G(d) basis set at the level of Moller-Plesset (MP) to second order. A complete vibrational assignment supported by normal coordinate calculations is proposed for the equatorial conformer, and several of the fundamentals of the axial conformer have also been identified. The results are discussed and compared to corresponding quantities for some similar molecules.