Alkali-metal atoms captured on the surface of superfluid helium droplets are excited to high energies (≈3 eV) by means of pulsed lasers, and their laser-induced-fluorescence spectra are recorded. We report on the one-photon excitation of the (n+1)p←ns transition of K, Rb, and Cs (n=4, 5, and 6, respectively) and on the two-photon one-color excitation of the 5d←5s transition of Rb. Gated-photon-counting measurements are consistent with the relaxation rates of the bare atoms, hence consistent with the reasonable expectation that atoms quickly desorb from the droplet and droplet-induced relaxation need not be invoked.

Visible absorption spectra of cesium-doped helium nanodroplets between 14,500 and 17,600 cm(-1) were probed by laser-induced fluorescence. A strong absorption band peaking around 16,700 cm(-1) is identified as Cs2 1(a) 3Sigmau+-3 3Sigmag+ transition. A broad unstructured band near 17,520 cm(-1) is assigned as the Cs2 1(X) 1Sigmag+-2 1Sigmau+ transition. Explanations of the observations are discussed on the basis of ab initio potential curves calculated by Spies and Meyer [(unpublished)]. All spectra have been modeled using narrow Frank-Condon windows around the equilibrium internuclear distance of the lowest singlet and triplet states. Many observed absorption peaks of smaller intensities could be identified, some of which may be due to transitions of cesium trimers formed on the droplets.

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