Homonuclear Decoupling of 1H Dipolar Interactions in Solids by means of Heteronuclear Recoupling

Abstract Line narrowing has been traditionally achieved in solid‐state 1H NMR spectroscopy by applying pulse sequences that combine multiple‐pulse operations with magic‐angle spinning (MAS), to effectively average out the dipoledipole homonuclear Hamiltonian. The present study explores a new alternative that departs from the usual concept of directly acting on the strongly coupled spins with radiofrequency pulses; instead, we seek to achieve a net homonuclear dipolar decoupling in solids by exploring the reintroduction of MAS‐averaged heteronuclear dipolar couplings between the 1H nuclei and directly bonded 13C or 15N nuclei. This recouplinganti‐recoupling (RaR) scheme thus relies on the recoupling of the dipolar interaction with heteronuclear spins, which, under fast MAS, will exceed the strength and will not commute with the homonuclear 1H1H coupling one is intending to average out. Subsequent removal (“antiRecoupling”) of these heteronuclear interactions can lead to narrowed 1H resonances, without ever pulsing on the aforementioned channel. The line‐narrowing properties of RaR are illustrated with numerical simulations and with experiments on model organic solids.