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Physical Review Letters

Rydberg States of Silver: Excitation Dynamics of Doped Helium Droplets

F. Federmann, Katrin Hoffmann, N. Quaas, J. D. Close

Published Sep 27, 1999• 37 citations
Publisher

Abstract

Silver atoms, initially embedded in nanodroplets of superfluid helium (roughly ${10}^{4}$ atoms in size), are found to move to the surface and desorb when excited to the broadened $5p$ level. The absorption of a second photon within less than 10 ns leads to the population of previously unobserved Rydberg states $(20<n<60)$ of free silver atoms. This is the first result showing laser induced movement of a foreign atom from the inside to the surface of a nanodroplet of superfluid helium.

DOI
10.1103/physrevlett.83.2548

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Silver atoms, initially embedded in nanodroplets of superfluid helium (roughly 104{10}^{4}104 atoms in size), are found to move to the surface and desorb when excited to the broadened 5p5p5p level. The absorption of a second photon within less than 10 ns leads to the population of previously unobserved Rydberg states (20<n<60)(20<n<60)(20<n<60) of free silver atoms. This is the first result showing laser induced movement of a foreign atom from the inside to the surface of a nanodroplet of superfluid helium.
Besides the use as cold matrix for spectroscopic studies, superfluid helium droplets have served as a cold environment for the synthesis of molecules and clusters. Since vibrational frequencies of molecules in helium droplets exhibit almost no shift compared to the free molecule values, one could assume the solvated particles move frictionless and undergo a reaction as soon as their paths cross. There have been a few unexplained observations that seemed to indicate cases of two species on one droplet not forming bonds but remaining isolated. In this work, we performed a systematic study of helium droplets doped with one rubidium and one strontium atom showing that besides a reaction to RbSr, there is a probability of finding separated Rb and Sr atoms on one droplet that only react after electronic excitation. Our results further indicate that ground-state Sr atoms can reside at the surface as well as inside the droplet.
Metal atoms have proved to be sensitive probes of the properties of superfluid helium nanodroplets. To date, all experiments on the doping of helium droplets have concentrated on the attachment of metal atoms in their ground electronic states. Here we report the first examples of metal atoms in excited states becoming attached to helium nanodroplets. The atoms in question are aluminum, and they have been generated by laser ablation in a metastable quartet state, which attaches to and remains on the surface of helium droplets. Evidence for a surface location comes from electronic spectra, which consist of very narrow absorption profiles that show very small spectral shifts. Supporting ab initio calculations show there to be an energy incentive for a metastable Al atom to remain on the surface of a helium droplet rather than move to the interior. The results suggest that helium droplets may provide a method for the capture and transport of metastable excited atomic and molecular species.
Superfluid helium nanodroplets provide a versatile substrate to cool atoms and molecules, and to assemble weakly bound complexes. Absence of spin-relaxation mechanisms makes He nanodroplets ideal to isolate open-shell atoms and create a spin-polarized system. Here, we show the first coherent manipulation of such a system by resonant excitation of a magnetic-dipole transition. Observation of approximately 50 Rabi oscillations demonstrates coherent population transfer with minimal dephasing. Ours is also the first application of ESR spectroscopy to doped He nanodroplets. This unique environment results in extremely sharp lines and hyperfine-resolved spectra: those of single 39K and 85Rb dopant atoms presented here denote an increase of the Fermi contact interaction, which we can follow as a function of droplet size, reflecting the distortion of the valence-electron wave function due to the surrounding He.
The desorption of excited rubidium atoms off the surface of helium nanodroplets is studied in detail using femtosecond time-resolved photoion and photoelectron imaging spectroscopy in combination with quantum wave-packet simulations. The good agreement of the measured time-dependent velocity distributions with the simulation when exciting the Rb dopant atoms into the 6p6p6p state supports the pseudodiatomic model for the Rb-He droplet interaction, even on the level of quantum wave-packet dynamics. Time-resolved photoelectron spectra reveal the partitioning of excitation energy into the dopant and the droplet degrees of freedom.