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Nuclear spins can be used as probes of electronic charge distribution by measuring frequencies of NMR transitions. Spins with $Ig\frac{1}{2}$ are particularly sensitive to the charge distribution through the nuclear quadrupole coupling. While classical magnetic resonance experiments monitor only electronic ground states, it is possible to investigate also electronically excited states by using optical-radio frequency double resonance techniques. We use Raman heterodyne spectroscopy to directly correlate NMR transitions from an electronically excited state to the corresponding transitions in the electronic ground state of the same system in a time-resolved two-dimensional experiment.

Correlating NQR transitions of ground and excited electronical states