Accelerating Structural Analysis: Decoding Homonuclear and Heteronuclear Chemical Shift Correlations in a Single Experiment at Fast MAS

Solid-state nuclear magnetic resonance (NMR) plays a vital role in the structural analysis of organic solids. Nevertheless, the intrinsically low sensitivity of solid-state NMR experiments often renders atomic-level structural determination challenging and time-consuming. Herein, by exhausting the 1H polarization under fast magic-angle-spinning conditions, we propose a pulse sequence enabling the acquisition of multiple-quantum/single-quantum (MQ/SQ) and 13C/1H chemical shift correlation spectra in a single experiment. Specifically, by implementation of the multiplex phase cycling schemes, MQ signals of different coherence orders in each transient scan can be well-separated and extracted. As a result, it is able to obtain 1H double-quantum/single-quantum (2Q/1Q), four-quantum/single-quantum (4Q/1Q), six-quantum/single-quantum (6Q/1Q), and 13C/1H chemical shift correlation spectra in a single experiment by fully utilizing the abundant 1H polarization following initial 1H–13C cross-polarization. We envisage that the current elegant pulse sequence design can inspire the development of novel solid-state NMR methodologies for speeding up the structural analysis of minute amounts of organic solids.