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The inherently low signal-to-noise ratio of NMR and MRI is now beingaddressed by hyperpolarization methods. For example, iridium-based catalyststhat reversibly bind both parahydrogen and ligands in solution canhyperpolarize protons (SABRE) or heteronuclei (X-SABRE) on a wide variety ofligands, using a complex interplay of spin dynamics and chemical exchangeprocesses, with common signal enhancements between $10^3-10^4$. This does notapproach obvious theoretical limits, and further enhancement would be valuablein many applications (such as imaging mM concentration species in vivo). MostSABRE/X-SABRE implementations require far lower fields (${\mu}T-mT$) thanstandard magnetic resonance (>1T), and this gives an additional degree offreedom: the ability to fully modulate fields in three dimensions. However,this has been underexplored because the standard simplifying theoreticalassumptions in magnetic resonance need to be revisited. Here we take adifferent approach, an evolutionary strategy algorithm for numericaloptimization, Multi-Axis Computer-aided HEteronuclear Transfer Enhancement forSABRE (MACHETE-SABRE). We find nonintuitive but highly efficient multi-axialpulse sequences which experimentally can produce a 10-fold improvement inpolarization over continuous excitation. This approach optimizes polarizationdifferently than traditional methods, thus gaining extra efficiency.

Multi-axis fields boost SABRE hyperpolarization via new strategies