Single and Double Resonance Microwave Spectroscopy in Superfluid $^4$He Clusters

Physics – Chemical Physics

Scientific paper

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4 pages, with 2 figures. To be published in Phys. Rev. Lett

Scientific paper

10.1103/PhysRevLett.82.5036

Purely rotational transitions of a molecule, such as HCCCN, embedded in large $^4$He 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 states of the inhomogeneous distribution of each rotational level, at a rate approximately 10 times faster than rotationally inelastic relaxation.

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