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                <term xml:lang="en">Rotaxanes</term>
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                <term xml:lang="en">Contrast agents</term>
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              <p>&lt;div&gt;&lt;p&gt;Rotaxanes and polyrotaxanes made of substituted cyclodextrins (CDs) were designed as potential MRI contrast agents or bimodal optical and MRI probes. After characterization of the threading kinetics and the exact composition of the polyrotaxanes, their MRI properties have been investigated by 1 H relaxometry and 17 O NMR. We demonstrated that the relaxivity of these systems is increasing with increasing size (modified CDs, rotaxanes, and polyrotaxanes). 17 O NMR studies show that the various systems have similar water exchange rates, in the same range as that of Gd-DOTA-monoamide complexes. Interestingly, NMRD data of the smaller systems can be only analyzed by considering both local and global motions via Lipari-Szabo approach, underlining the importance of internal flexibility. On the other hand, the disubsituted rotaxane and the polyrotaxanes are highly rigid and can be characterized with a single rotational correlation time. Their relaxivity is considerably enhanced by a second sphere contribution which is strongly dependent on the structure. It increases from the rotaxane to the mono-and the disubstituted polyrotaxanes, and as expected, it diminishes with decreasing coverage of the axle. The fundamental understanding provided by this comprehensive study will help the design of versatile and more efficient supramolecular interlocked systems such as rotaxanes and polyrotaxanes for MRI applications.&lt;/p&gt;&lt;/div&gt;</p>
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