Nuclear Magnetic Resonance of Hydrogen Molecules Trapped inside C(70) Fullerene Cages

We present a solid-state NMR study of H(2) molecules confined inside the cavity of C(70) fullerene cages over a wide range of temperatures (300 K to 4 K). The proton NMR spectra are consistent with a model in which the dipole–dipole coupling between the ortho-H(2) protons is averaged over the rotational/translational states of the confined quantum rotor, with an additional chemical shift anisotropy δ(H)(CSA)=10.1 ppm induced by the carbon cage. The magnitude of the chemical shift anisotropy is consistent with DFT estimates of the chemical shielding tensor field within the cage. The experimental NMR data indicate that the ground state of endohedral ortho-H(2) in C(70) is doubly degenerate and polarized transverse to the principal axis of the cage. The NMR spectra indicate significant magnetic alignment of the C(70) long axes along the magnetic field, at temperatures below ∼10 K.