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Molecular reorientation of CD4 in gas‐phase mixtures

Spin‐lattice relaxation times were measured for the deuterons in CD4 in pure gas and in mixtures with the following buffer gases: Ar, Kr, Xe, HCl, N2, CO, CO2, CF4, and SF6. Effective collision cross sections σθ, 2 for the molecular reorientation of CD4 in collisions with these ten molecules are obtained as a function of temperature. These cross sections are compared with the corresponding cross sections σJ obtained from 1H spin‐rotation relaxation in mixtures of CH4 with the same set of buffer gases. Various classical reorientation models typically applied in liquids predict different ratios of the reduced correlation times for the reorientation of spherical tops. The Langevin model comes closest to predicting the magnitude of the σθ, 2/σJ ratio that we obtain for CD4. Copyright © 2006 John Wiley & Sons, Ltd.