1H and 19F ultra-fast MAS double-quantum single-quantum NMR correlation experiments using three-spin terms of the dipolar homonuclear Hamiltonian

Measuring internuclear distances through dipolar interaction is a major challenge for solid-state nuclear magnetic resonance (NMR) spectroscopy. Obtaining reliable interatomic distances provides an access to the local structure in ordered or disordered solids. We show that at magic angle spinning (MAS) frequencies larger than ca. 50 kHz, some of the three-spin terms of the homogeneous homonuclear dipolar Hamiltonian can be used to promote the creation of double-quantum coherences between neighbouring (1)H or (19)F spins without using dipolar recoupling pulse sequences in the Dipolar Homonuclear Homogeneous Hamiltonian (DH(3)) double-quantum/single-quantum correlation experiment. This makes it possible to probe inter-nuclear spatial proximity with limited risk of probe or sample damage from radio-frequency (RF) irradiation, and is fully appropriate for fast repetition rate offering sensitivity gains in favourable cases. Experimental demonstrations are supported by multi-spin numerical simulations, which points to new possibilities for the characterization of spin-system geometries.