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Abstract
The anisotropic motional behavior of an isolated two-spin system is investigated via NMR relaxation measurements. Complete description of anisotropic rotational diffusion is possible if the CSA mechanism contributions to the relaxation and cross correlations between dipolar interactions and chemical-shift anisotropy are included. Various pulse experiments together with diverse cross checks are employed to derive unambiguous results. In addition these cross terms allow the determination of the absolute sign of the indirect coupling constant.
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