Heterodyne spectral interferometry for multidimensional nonlinear spectroscopy of individual quantum systems

A novel implementation of transient nonlinear spectroscopy is presented that allows the study of the transient nonlinear polarization emitted from individual electronic transitions. Both the amplitude and the phase of the polarization are retrieved, permitting the implementation of multidimensional spectroscopy in the excitation pulse delays. The technique is shown to detect mutual coherent coupling in a group of individual, localized excitonic transitions.