Abstract Modern NMR methods in liquids are based on the transfer of polarisation from nucleus to nucleus to generate multidimensional heteronuclear correlation spectra. The factors that influence the efficiency of heteronuclear polarisation transfer in multi-pulse experiments, and in that way the quality of spectra are the subject of this thesis. The flow of coherence through pulse sequences can be designed and analysed with the aid of product operator calculations. Results of the study include improvements to quantitative two-dimensional shift-correlated experiments, and demonstration of the benefits of closely spaced 180° pulse trains in polarisation transfer steps in long-range correlation experiments and isotope editing filters.