Homonuclear dipolar decoupling with very large scaling factors for high-resolution ultrafast magic angle spinning 1H solid-state NMR spectroscopy

► Introducing a new class of homonuclear dipolar decoupling experiments for solid-state NMR using very fast magic angle sample spinning, which are well out of the traditional CRAMPS regime, and which provide the best experimental decoupling performance to date. ► The sequences were found through a novel optimization strategy using directly the proton NMR spectrum for the first time. ► The sequences have a scaling factor that is larger than that possible in the static limit. This is what yields their high performance. ► It is confirmed that the sequences operate in a joint averaging regime.