Measurements of spin-lattice relaxation, combined with 2-dimensional measurements of single-and double-quantum spin-echo decay rates, were used to detn. the complete set of spectral d. parameters which characterize D relaxation of CD2Cl2 partially oriented in a nematic liq. crystal (Merck Licristal Phase V). At 31.5 Deg and 9.2 MHz, terms describing cross-correlation between 2 D quadrupole coupling tensors are comparable to the autocorrelation terms. A partial interpretation of these results in terms of anisotropic mol. reorientation and order-director fluctuations is presented and is confirmed by addnl. measurements of the temp. and field dependence of spin-lattice relaxation rates. [on SciFinder (R)]