Generalised magnetisation-to-singlet-order transfer in nuclear magnetic resonance

A variety of pulse sequences have been described for converting nuclear spin magnetisation into long-lived singlet order for nuclear spin-1/2 pairs. Existing sequences operate well in two extreme parameter regimes. The magnetisation-to-singlet (M2S) pulse sequence performs a robust conversion of nuclear spin magnetisation into singlet order in the near-equivalent limit, meaning that the difference in chemical shift frequencies of the two spins is much smaller than the spin-spin coupling. Other pulse sequences operate in the strong-inequivalence regime, where the shift difference is much larger than the spin-spin coupling. However both sets of pulse sequences fail in the intermediate regime, where the chemical shift difference and the spin-spin coupling are roughly equal in magnitude. We describe a generalised version of M2S, called gM2S, which achieves robust singlet order excitation for spin systems ranging from the near-equivalence limit well into the intermediate regime. This closes an important gap left by existing pulse sequences. The efficiency of the gM2S sequence is demonstrated numerically and experimentally for near-equivalent and intermediate-regime cases.