Raman magnetic resonance where double-quantum transitions are observed with
out the need for multidimensional n.m.r. spectroscopy has been investigated
further. Theoretical analysis of the on-resonance case where weak continuo
us-wave irradiation was applied at the frequency of a single-quantum transi
tion was performed and guidelines for a consistent perturbation treatment w
ere devised. Theoretical results agree well with experimental data obtained
for a system of two dipolar coupled nuclei of spin 1/2 oriented by a liqui
d crystal. The same approach is applicable to near-resonance experiments wh
ich are shown to be the optimal experimental scheme for Raman n.m.r. By usi
ng weak selective irradiation, a symmetric excitation-detection scheme can
be realized for multiple-quantum n.m.r. experiments. Near- or on-resonance
selective irradiation provides an efficient transfer of multiquantum cohere
nce into observable coherences and could be used to study multiquantum rela
xation processes.