Multiaxial fields improve SABRE efficiency by preserving hydride order

• Multiaxial field geometries expand control over SABRE hyperpolarization. • CW decoupling on a perpendicular axis preserves singlet for polarization transfer. • Polarization transfer at SABRE SHEATH conditions is improved by 2.5-fold. Signal Amplification By Reversible Exchange (SABRE) and the heteronuclear variant, X-SABRE, increase the sensitivity of magnetic resonance techniques using order derived from reversible binding of para -hydrogen. One current limitation of SABRE is suboptimal polarization transfer over the lifetime of the complex. Here, we demonstrate a multiaxial low-field pulse sequence which allows optimal polarization build-up during a low-field “evolution” pulse, followed by a high-field “mixing” pulse which permits proton decoupling along an orthogonal axis. This preserves the singlet character of the hydrides while allowing exchange to replenish the ligands on the iridium catalyst. This strategy leads to a 2.5-fold improvement over continuous field SABRE SHEATH experimentally which was confirmed with numerical simulation.