Decoupled LIGHT-SABRE variants allow hyperpolarization of asymmetric SABRE systems at an arbitrary field

[Display omitted] •SABRE at high field is restricted to symmetric ligand environments.•1H-decoupled LIGHT-SABRE variants expand the scope to targets requiring co-ligands.•Ligand binding competition is measured between co-ligand and target. Signal Amplification By Reversible Exchange, or SABRE, uses the singlet-order of parahydrogen to generate hyperpolarized signals on target nuclei, bypassing the limitations of traditional magnetic resonance. Experiments performed directly in the magnet provide a route to generate large magnetizations continuously without having to field-cycle the sample. For heteronuclear SABRE, these high-field methods have been restricted to the few SABRE complexes that exhibit efficient exchange with symmetric ligand environments as co-ligands induce chemical shift differences between the parahydrogen-derived hydrides, destroying the hyperpolarized spin order. Through careful consideration of the underlying spin physics, we introduce 1H decoupled LIGHT-SABRE pulse sequence variants which bypasses this limitation, drastically expanding the scope of heteronuclear SABRE at high field.