Single and double resonance microwave spectroscopy in superfluid 4He clusters

Purely rotational transitions of a molecule embedded in large He-4 clusters have been detected for the first time. The saturation behavior shows that, in contrast to previous expectations, the microwave line profiles are dominated by inhomogeneous broadening mechanisms. Spectral holes and peaks produced by microwave-microwave double resonance have widths comparable to those of single resonance lines, indicating that relaxation occurs among quantum slates of the inhomogeneous distribution of each rotational level, at a rate approximate to 10 times faster than rotationally inelastic relaxation.