AbstractThe translational and orientational dynamics of water in carbon nanotubes has been studied by quasi-elastic neutron scattering from 300 down to 10 K. Results show that, reducing temperature below 200 K, part of this water behaves as a quasi-free rotor, that is, the orientational energy of such molecules becomes comparable to the rotational energy of water in the gas phase. This novel and unique dynamic behavior is related to the appearance of water molecules characterized by a coordination number of about two, which is promoted by sub-nanometer axial confinement. This peculiar molecular arrangement allows water to show an active rotational dynamics even at temperatures as low as 10 K. The translational mobility shows a behavior compatible with the rotational one.