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Zeitschrift für Physik D Atoms Molecules and Clusters

Magnetic properties of free alkali and transition metal clusters

Walt A. de Heer, P. Milani, A. Châtelain

Published Mar 1, 1991• 33 citations
Publisher
DOI
10.1007/bf01448302

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The study of small clusters is intended to fill the knowledge gap between single atoms and bulk material. He nanodroplets are an ideal matrix for preparing and investigating clusters in a superfluid environment. Alkali-metal atoms are only bound very weakly to their surface by van der Waals forces. Due to the formation process, high-spin states of alkali-metal clusters on He nanodroplets are favorably observed, which is in contrast to the abundance in other preparation processes. Until now, the prevailing opinion was that stable clusters of the heavy alkali-metal atoms, rubidium (Rb) and cesium (Cs) on He nanodroplets, are limited to 5 and 3 atoms, respectively (Schulz et al., Phys. Rev. Lett. 2004, 92, 13401). Here, we present stable complexes of Rb(n)⁺ and Cs(n)⁺ consisting of up to n = 30 atoms, with the detection of large alkali-metal clusters being strongly enhanced by one-photon ionization. Our results also suggest that we monitored both high-spin and low-spin state clusters created on nanodroplets. The van der Waals bound high-spin alkali-metal clusters should show strong magnetic behavior, while low-spin states are predicted to exhibit metallic characteristics. Alkali-metal clusters prepared in these two configurations appear to be ideal candidates for investigating nanosized particles with ferromagnetic or metallic properties.
By use of a free-energy model, the properties of a fluid composed of neutral atoms and diatomic molecules, positive ions and molecular ions, and an electron Fermi gas are calculated. The interactions include excluded volume, internal molecular binding, electron-neutral s-wave scattering, and screened Hartree interactions. For rubidium and cesium parametrizations, the vapor-liquid phase transitions with their critical points, the insulator-metal transitions, and the isothermal electrical conductivities and magnetic susceptibilities are obtained.
The probabilities of atomic transitions F e − F g = ± 2 between a ground F g and an excited F e level of the D 2 line of any alkali metal atom are zero when no external magnetic field is applied. In an external magnetic field in the range of 0.1–3 kG, the probabilities of these transitions called magnetically induced (MI) are highly modified. For MI transitions, we previously exhibited the following rule: the probabilities of MI transitions with Δ F = + 2 are maximal when using σ + -polarized laser radiation, while the probabilities of MI transitions with Δ F = − 2 are maximal when using σ − -polarized laser radiation. This difference has been termed type 1 MI circular dichroism. It is demonstrated for the first time, to our knowledge, that for alkali atoms with a nuclear spin I = 3 / 2 ( 87 R b , 39 K , 23 N a , 7 L i ) in magnetic fields > 100 G , the probability of the strongest σ + MI transition of the group F g = 1 → F e = 3 ′ (transition | 1 , − 1 ⟩ → | 3 ′ , 0 ′ ⟩ ) is about four times higher than the probabilities of the strongest MI σ − -transitions | 1 , − 1 ⟩ → | 3 ′ , − 2 ′ ⟩ and | 2 , + 1 ⟩ → | 0 ′ , 0 ′ ⟩ . These properties make the σ + MI transition | 1 , − 1 ⟩ → <m