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We describe a new method for pulsed spin order transfer (SOT) of parahydrogeninduced polarization (PHIP) that enables close to 100 % polarization inincompletely 2H-labeled molecules by exciting only the desired protons in afrequency-selective manner. While a selective pulse (SP) on 1H at the beginningof pulsed SOT had been considered before, using SPs during the SOT suppressesundesired indirect spin-spin interactions. As a result, we achieved a morerobust SOT for the SP variants of the phINEPT+ sequence that we refer to asphSPINEPT+. Thereby, for the first time, we report a sequence that is effectivefor all weakly coupled spin systems. Our simulations show that the methodconverts close to 100 % of the parahydrogen-derived spin order into 13Chyperpolarization in weakly coupled three-spin systems and partially or fully2H-labeled molecules if relaxation is neglected. Experimentally we demonstratehigh hyperpolarization of 13C with 15.8 % for 1-13C-hydroxyethyl propionate-d3and 12.6 % for 1-13C-ethyl acetate-d6, which corresponds to ~47 % and ~38 % ifthe enrichment of parahydrogen had been 100 %. Even in non-2H-labeledmolecules, a remarkable 13C polarization is achieved, e.g. up to 20 % weresimulated for 100 % pH2, and 1.25 % were obtained experimentally for1-13C-ethyl pyruvate and 50 % pH2, which can be further improved by fasterhydrogenation. As a result, full deuterium labeling may no longer be requirede.g., when new PHIP agents are investigated, the synthesis of fully deuteratedmolecules is too complex, or when a kinetic isotope effect regarding themetabolic conversion rate of an agent is to be avoided. Using SPs during SOTseems very promising and may be extended to other sequences in the context ofPHIP and be-yond to make them less prone to experimental imperfections or realmolecular environments.

Selectively pulsed spin order transfer increases parahydrogen-induced  NMR amplification of insensitive nuclei and makes polarization transfer more  robust