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Most theoretical models for NMR relaxation in liquids assume that overall rotational motion can be described as rotational diffusion with a single diffusion tensor. Such models cannot handle motions (such as between "closed" and "open" states of an enzyme, or between conformers of a partially disordered system) where the shape of the molecule (and hence its rotational diffusion behavior) fluctuates. We provide here a formalism for dealing with such problems. The model involves jumps between discrete conformers with different overall diffusion tensors, and a master (rate) equation to describe the transitions between these conformers. Numerical examples are given for a two-site jump model where global and local motions are concerted, showing how the rate of conformational transitions (relative to the rate of rotational diffusion) affects the observed relaxation parameters.

Influence of the coupling of interdomain and overall motions on NMR relaxation