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Register a new userFission of Multiply Charged Cesium and Potassium Clusters in Helium Droplets - Approaching the Rayleigh Limit
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Electron ionization of helium droplets doped with cesium or potassium results in doubly and, for cesium, triply charged cluster ions. The smallest observable doubly charged clusters are $Cs_{9}^{2+}$ and $K_{11}^{2+}$; they are a factor two smaller than reported previously. The size of potassium dications approaches the Rayleigh limit nRay for which the fission barrier is calculated to vanish, i.e. their fissilities are close to 1. Cesium dications are even smaller than nRay, implying that their fissilities have been significantly overestimated. Triply charged cesium clusters as small as $Cs_{19}^{3+}$ are observed; they are a factor 2.6 smaller than previously reported. Mechanisms that may be responsible for enhanced formation of clusters with high fissilities are discussed.
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We report on the production and study of stable, highly charged droplets of superfluid helium. Using a novel experimental setup we produce neutral beams of liquid helium nanodroplets containing millions of atoms or more that can be ionized by electron impact, mass-per-charge selected, and ionized a second time before being analyzed. Droplets containing up to 55 net positive charges are identified and the appearance sizes of multiply charge droplets are determined as a function of charge state. We show that the droplets are stable on the millisecond time scale of the experiment and decay through the loss of small charged clusters, not through symmetric Coulomb explosions.
The surface composition of charged Lennard-Jones clusters A$_N^{n+}$, composed of N particles (55 leq N leq 1169) among which n are positively charged with charge q, thus having a net total charge Q = nq, is investigated by Monte Carlo with Parallel Tempering simulations. At finite temperature, the surface sites of these charged clusters are found to be preferentially occupied by charged particles carrying large charges, due to Coulombic repulsions, but the full occupancy of surface sites is rarely achieved for clusters below the stability limit defined in this work. Large clusters (N = 1169) follow the same trends, with a smaller propensity for positive particles to occupy the cluster surface at non-zero temperature. We show that these charged clusters rather behave as electrical spherical conductors for the smaller sizes (N leq 147) but as spheres uniformly charged in their volume for the larger sizes (N = 1169).
The mechanism of ionization of helium droplets has been investigated in numerous reports but one observation has not found a satisfactory explanation: How are $He^+$ ions formed and ejected from undoped droplets at electron energies below the ionization threshold of the free atom? Does this path exist at all? A measurement of the ion yields of $He^+$ and $He_2^+$ as a function of electron energy, electron emission current, and droplet size reveals that metastable $He^{*-}$ anions play a crucial role in the formation of free $He^+$ at subthreshold energies. The proposed model is testable.
We report the first observation of cations, dications and trications of large clusters of adamantane. Cluster formation was initiated near 0 K in helium droplets and ionization was achieved with one or more collisions with energetic He species (He$^{star}$, He$^{+}$ or He$^{star}$$^{-}$). The occurrence of Coulomb explosion appeared to discriminate against the formation of small multiply charged clusters. High resolution mass spectrometry revealed the presence of magic number m/z peaks that can be attributed to the packing of adamantane molecules into cluster structures of special stability involving preferred arrangements of these molecules. These abundance anomalies were seen to be independent of charge state. While some dehydrogenation of adamantane and its clusters was seen as well, no major transformations into adamantoids or microdiamonds were observed.
We propose a method for quantifying charge-driven instabilities in clusters, based on equilibrium simulations under confinement at constant external pressure. This approach makes no assumptions about the mode of decay and allows different clusters to be compared on an equal footing. A comprehensive survey of stability in model clusters of 309 Lennard-Jones particles augmented with Coulomb interactions is presented. We proceed to examine dynamic signatures of instability, finding that rate constants for ejection of charged particles increase smoothly as a function of total charge with no sudden changes. For clusters where many particles carry charge, ejection of individual charges competes with a fission process that leads to more symmetric division of the cluster into large fragments. The rate constants for fission depend much more sensitively on total charge than those for ejection of individual particles.
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