Systems and methods are disclosed for increasing a nuclear spin polarization of a target compound. In accordance with such systems and methods, a first non-thermal equilibrium nuclear spin polarization can be imparted to at least one source atom of a source compound, the source atom having a nuclear gyromagnetic ratio of at least 12 megahertz per tesla (MHz/T). A first solution can be obtained that includes the source compound and a target compound. The at least one source atom can be present in a source concentration of at least 0.1 molar (M) in the first solution. A second non-thermal equilibrium nuclear spin polarization of at least 0.01% can be imparted to the at least one target atom of the target compound via a nuclear Overhauser effect (NOE) transfer of the first non-thermal equilibrium nuclear spin polarization to the at least one target atom.