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Spectroscopy of Alkali Atoms and Molecules Attached to Highly Quantum Clusters

Frank Stienkemeier, John P. Higgins, Wolfgang Ernst, Carlo Callegari, G. Scoles

Published Jun 11, 1995• 0 citations
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Spectroscopy of doped helium nanodroplets has become, in recent years, a popular tool for the study of bothfinite size samples of the helium quantum fluid and molecules isolated in this sub Kelvin environment. Whilemany dopants migrate to the center of the droplet, alkali (Ak) atoms in their ground electronic state, becauseof their so weak interaction with He, remain at the surface, the latter being in this way slightly distortedexhibiting a dimple. However, when in their first excited states, Ak atoms are forming exciplexes. These areanisotropic with the central atom surrounded by a ring of He atoms located in the nodal plane of the valenceelectron pz orbital. Structural properties, obtained by DMC and PIMC, are presented here for some Ak -Hen exciplexes.Ak2 dimers in helium environment have also gained interest in this last decade, in connexion with the generationof ultracold molecules. When attached to helium droplets, Ak atoms can float on the surface andform molecules in cold collisions. DMC and PIMC methods are used to compute energetics and structuralinformations for Rb2 in helium. In particular, the orientation of the dimer relative to the droplet surface isexamined.

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Helium clusters and droplets: microscopic superfluidity and other quantum effects†

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Many microscopic properties of the only natural superfluid element helium have become available within the last 18 years through a number of novel experiments. The diffraction of matter-waves of small helium clusters has established the unusually large bond distance (5.2 nm) and extremely weak binding energy (10−7 eV) of the dimer and other exotic properties of small helium clusters. The high-resolution spectroscopy of closed-shell chromophore molecules attached to small clusters or embedded inside large superfluid droplets have revealed that as a result of superfluidity, molecules rotate virtually without friction and that only a handful of He atoms are required for microscopic superfluidity. The frictionless translational motion of atoms and molecules inside the droplets has also been observed. These and a number of other experiments demonstrate that helium droplets are the most gentle and coldest of all cryomatrices with enormous potential for a wide range of future applications.

Molecular Physics•Jun 14, 2013•48 citations
Spectroscopy of doped helium nanodroplets has become, in recent years, a popular tool for the study of bothfinite size samples of the helium quantum fluid and molecules isolated in this sub Kelvin environment. Whilemany dopants migrate to the center of the droplet, alkali (Ak) atoms in their ground electronic state, becauseof their so weak interaction with He, remain at the surface, the latter being in this way slightly distortedexhibiting a dimple. However, when in their first excited states, Ak atoms are forming exciplexes. These areanisotropic with the central atom surrounded by a ring of He atoms located in the nodal plane of the valenceelectron pz orbital. Structural properties, obtained by DMC and PIMC, are presented here for some Ak -Hen exciplexes.Ak2 dimers in helium environment have also gained interest in this last decade, in connexion with the generationof ultracold molecules. When attached to helium droplets, Ak atoms can float on the surface andform molecules in cold collisions. DMC and PIMC methods are used to compute energetics and structuralinformations for Rb2 in helium. In particular, the orientation of the dimer relative to the droplet surface isexamined.
Many microscopic properties of the only natural superfluid element helium have become available within the last 18 years through a number of novel experiments. The diffraction of matter-waves of small helium clusters has established the unusually large bond distance (5.2 nm) and extremely weak binding energy (10−7 eV) of the dimer and other exotic properties of small helium clusters. The high-resolution spectroscopy of closed-shell chromophore molecules attached to small clusters or embedded inside large superfluid droplets have revealed that as a result of superfluidity, molecules rotate virtually without friction and that only a handful of He atoms are required for microscopic superfluidity. The frictionless translational motion of atoms and molecules inside the droplets has also been observed. These and a number of other experiments demonstrate that helium droplets are the most gentle and coldest of all cryomatrices with enormous potential for a wide range of future applications.