Rapid Structural Analysis of Minute Quantities of Organic Solids by Exhausting 1 H Polarization in Solid-State NMR Spectroscopy Under Fast Magic Angle Spinning.

Solid-state nuclear magnetic resonance (NMR) often suffers from significant limitations due to the inherent low signal sensitivity when low-γ nuclei are involved. Herein, we report an elegant solid-state NMR approach for rapid structural analysis of minute amounts of organic solids. By encoding staggered chemical shift evolution in the indirect dimension and staggered acquisition in the 1 H dimension, a proton-detected homonuclear 1 H/ 1 H and heteronuclear 13 C/ 1 H chemical shift correlation (HETCOR) spectrum can be obtained simultaneously in a single experiment at a fast magic-angle-spinning (MAS) condition with barely increasing the experimental time. We further show that during the conventional 1 H-detected HETCOR experimental time, multiple homonuclear 1 H/ 1 H correlation spectra can be recorded in addition to the HETCOR spectrum, enabling the determination of 1 H- 1 H distances. We establish that abundant 1 H polarization can be efficiently manipulated and fully utilized in proton-detected solid-state NMR spectroscopy for extraction of more critical structural information and thus reduction of the total experimental time.