An NMR pulse sequence was designed to accurately measure the diffusion rate
s of intermolecular zero-quantum coherences (ZQCs) and double-quantum coher
ences (DQCs) in two-component spin systems. The Gaussian phase distribution
approximation was employed to describe the behavior of intermolecular ZQCs
and DQCs as they underwent unrestricted isotropic diffusion. Our experimen
tal and theoretical results demonstrate that intermolecular ZQCs and DQCs e
volve with the same diffusion rates. Uncorrelated phases between individual
spins on different molecules in intermolecular ZQCs and DQCs are suggested
as the cause for their unconventional diffusion behavior. The differences
in diffusion rates between inter- and intramolecular ZQCs or DQCs are expla
ined. (C) 2001 Elsevier Science B.V. All rights reserved.