Nuclear spin conversion of methane in pure and rare-gas mixed crystals

Spin species conversion has been observed by means of neutron scattering. Methane, matrixisolated in rare-gas crystals has been investigated by measuring the time dependence of the detailed balance factor of inelastic neutron spectra. The temperature dependence of conversion rates in the interval between 2 and 5 K turns out to be stronger than predicted by a single phonon process. In general, conversion times are of the order of hours in this temperature region. The influence of the matrix is well described by a coupled phonon density of states. Crystals of pure and krypton doped methane have been examined by measuring the time dependence of the total neutron scattering cross section. For pure methane, the temperature dependence of the conversion rates shows two regimes for both free rotator and ordered molecules. Below 5 K, the behavior is described by a single phonon process and above by an Arrhenius law. Rates are enhanced by krypton dotation, which is explained by changed level spacings due to orientational disorder.