The highly anisotropic spin–lattice relaxation times in pure nuclear quadrupole resonance of 14N in piperazine are investigated in terms of anisotropic molecular rotations with respect to the principal axes of the electric‐field‐gradient tensor. A sudden approximation is used to obtain relations between the geometrical parameters of the molecular rotations and the correlation time involved. The double resonance technique is used to determine the relaxation times of the three‐energy‐level system.

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