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The internal hollow space of carbon nanotubes provides a unique nanometre-sized space to capture various molecular entities. The inner space circumfused by sp 2 -carbon networks can also encapsulate diamondoid molecules to afford sp 2 /sp 3 -hybrid nanocarbon peapods that have recently emerged as unique nanostructures. In this study, the sp 2 /sp 3 -hybrid peapods have been mimicked by adopting a cylindrical molecule and the smallest diamondoid, i.e., adamantane, to demonstrate the existence of ultrafast rotational motion. The solid-state rotational frequency is measured by NMR spectroscopy to record 1.06 THz that is, to the best of our knowledge, the largest value recorded for solid-state rotations of molecules. Theoretical calculations reveal that multivalent CH-π hydrogen bonds anchored the diamondoid guest on the π-wall of the cylindrical host. The weak hydrogen bonds are prone not only to cleave but also to regenerate at the interfaces, which give freedom to the guest for ultrafast isotropic rotations in the inertial regime.

A hybrid molecular peapod of sp2- and sp3-nanocarbons enabling ultrafast terahertz rotations