Phase separation into pure components in mixed Ar-Xe clusters

Phase equilibrium in binary clusters of heavy inert gases has been studied using a combination of electron diffraction and optical methods. Mixed Ar-Xe clusters exhibit the phenomenon of phase separation into pure components with the formation of a sharp interface between the xenon core and argon shell, which is not observed in massive samples of this system.     

Formation of mixed clusters in a pulsed supersonic helium-oxygen-isoprene jet

An experimental study of the formation of mixed van der Waals oxygen-isoprene complexes, generated in an expanding supersonic helium-oxygen-isoprene jet at various stagnation pressures and at diverse oxygen and isoprene concentrations, has been performed. To measure the composition and distribution of the partial densities of the individual components, molecular beam mass spectrometry was adapted to pulsed modes of gas source operation. The particularities of applying mass spectrometry to studying clustered isoprene streams in a pulsed mode have been discussed. The composition of small clusters generated in a free supersonic jet has been checked for dependencies upon the initial mixture composition and stagnation pressure. The mechanism of nucleation has been identified for different partial concentrations of impurities in the helium stream. It has been shown that, even at a 0.3% concentration of isoprene in the mixture, nucleation starts with the formation of hydrocarbon complexes. The specific features of the dissociative ionization of van der Waals complexes, consisting of pure isoprene and mixed complexes, have been discussed. The conditions needed for the formation of binary oxygen-isoprene van der Waals complexes have been identified.     

Interpretation of a repulsive core between fermion clusters

The notion of relative distance between two composite fermion clusters, such as nucleons in a quark model, is ambiguous at small separations. We examine the consequences of defining relative distance as the largest relative coordinate of all possible clusterings of the constituent particles. Such a definition can naturally yield a repulsive core in the effective potential between the two composite systems.     

常温下氙气以及氢氙混合气体形成的团簇的特性研究

利用瑞利散射法可以对团簇的尺寸以及团簇形成的演变过程进行研究, 这种方法非常简单易行且对团簇是非破坏性的. 通过对纯氙气以及氢氙混合气体形成的团簇的瑞利散射进行测量, 研究并分析了瑞利散射强度随时间、初始背压 以及气体混合比例的变化, 由此估算了在不同情况下形成团簇的平均尺寸. 通过获得的氢氙混合气体瑞利散射强度与背压的关系I=(1.5 ×10^-5)P^6.47, 发现了混合气体中氢气对氙团簇形成的促进作用, 并从热力学和分子间作用力的角度进行了理论分析, 得到了氢氙混合气体不易于液化这一新现象, 为实现高背压下更大尺寸团簇的产生提供了可能. 所获得的结果为今后基于氙团簇的X射线产生实验, 以及基于氘氙混合气体的中子产生实验研究提供了良好的实验依据.     

Anions of xenon clusters bound by long-range electron correlations

In contrast with the single atom, atomic van der Waals clusters can form stable anions where the excess electron is bound due to long-range correlations with the electrons of the cluster. We report on extensive all-electron many-body ab initio studies on Xe clusters. Three-dimensional, planar, and linear structures of the clusters are investigated and compared. In particular, we find that the minimal number of Xe atoms in the cluster required to form a stable anion is 5 independently of the dimensionality of the cluster. We provide electron affinities for clusters made of 5, 6, and 7 atoms in all dimensions and find that the planar clusters form the most stable anions. The Dyson orbitals of the excess electrons are computed and analyzed.     

Formation of polaron clusters

The formation of spherical polaron clusters is studied within the Fröhlich polaron theory. In a dilute polaron gas, using the non-local statistical approach and the polaron pair interaction obtained within the Pekar strong coupling theory, the homogeneous phase results to be unstable toward the appearance of polaron clusters. The physical conditions of formation for the clusters are determined calculating the critical values of electron-phonon interaction for which bound states in the collective polaron potential develop. Finally the sequence in the filling of the states is found and the stability of the clusters is assessed.Received: 6 May 2004, Published online: 12 October 2004PACS: 71.38.-k Polarons and electron-phonon interactions     

Electronic properties of mixed lithium-oxygen clusters

Herein electronic structure as a function of cluster size has been probed through ionization potentials measurements in order to derive general trends in the evolution of the structure and stability of lithium oxide clusters LinOm. The structural evolution was investigated by varying progressively the oxygen rate in order to observe transitions from the metallic Lin to the ionic structure (Li2O)n. We have demonstrated that this structural transition splits into three specific ranges. This result, in contrast with the general behavior observed with other electronegative elements combined with alkaline or alkaline-earth metal clusters, but similar to what is known about BanOm and CsnOm, constitutes a signature of a specific role played by the oxygen atoms when included inside a metallic cluster.     

The structure of mixed nitrogen-argon clusters

Using realistic pair potentials, we investigate the structures of mixed clusters of argon and nitrogen in order to interpret the experimental electron diffraction patterns reported by the Torchet group. Simulations of small clusters indicate that argon tends to segregate at the center of the clusters. For larger clusters, in the range of 50 to 200 molecules, MC methods have been used to simulate structures that are likely to be generated in the molecular beam. By comparing predicted electron diffraction patterns with those recorded in the experiments, our models allow us to estimate the average size and composition of the mixed clusters for a given set of experimental conditions (nozzle stagnation pressure and Ar partial pressure).     

Enhancement of double auger decay probability in xenon clusters irradiated with a soft-x-ray laser pulse

The interaction of large Xe clusters with a soft x-ray laser pulse having a wavelength of 13.9 nm and an intensity of up to 2x10(10) W/cm2 was investigated using a time-of-flight ion mass spectrometer. The corresponding laser photon energy was sufficiently high to photoionize Xe 4d innershell electrons. It was found that Xe3+ ions (which result from double Auger decay of 4d vacancies) became the dominant final ionic product with increasing cluster size and x-ray intensity. This is in contrast to the results of synchrotron radiation experiments involving free Xe atoms, in which Xe2+ is the dominant resultant ion species. Possible mechanisms responsible for the enhancement of the double Auger transition probability in x-ray laser and cluster interaction are discussed.     

Spectroscopy of calcium deposited on large argon clusters

Spectroscopic experiments have been performed, providing emission and excitation spectra of calcium atoms trapped on argon clusters of average size 2 000. The two experimental spectra fall in the vicinity of the calcium resonance line ¹P ₁ → ¹S₀ at 422.9 nm. The excitation spectrum consists in two bands located on each side of the resonance line of the free calcium. In addition, Monte Carlo calculations, coupled to Diatomics-In-Molecule potentials are employed to simulate the absorption spectrum of a single calcium atom in the environment of a large argon cluster of average size 300. The theoretical absorption spectrum confirms the existence of two bands, and shows that these bands are characteristic of a calcium atom located at the surface of the argon cluster and correspond to the excited 4p orbital of calcium either perpendicular or parallel to the cluster surface. The precise comparison between the shape of the absorption spectrum and that of the fluorescence excitation spectrum shows different intensity ratios. This could suggest the existence of a non adiabatic energy transfer that quenches partly the fluorescence of trapped calcium. Another explanation, although less likely, could be a substantial dependence of the calcium oscillator strength according to the alignment of the calcium excited orbital with respect to the cluster surface. The emission spectrum always shows a band in the red of the resonance line which is assigned to the emission of calcium remaining trapped on the cluster. When exciting the blue band of the excitation spectrum, the emission spectrum shows a second, weak, component that is assigned to calcium atoms ejected from the argon clusters, indicating a competition between ejection and solvation. Received 7 May 2002 Published online 1st October 2002 RID="a" ID="a"e-mail: jmm@drecam.saclay.cea.fr RID="b" ID="b"URA 2453 du CNRS RID="c" ID="c"UMR 5626 du CNRS     

Diagnostics of mixed van der Waals clusters

We present two complementary techniques that provide detailed diagnostics of supersonic beams involving several species. First, surface scattering, together with quadrupole mass spectrometer detection, yields the monomer percentage for each species within the beam. Second, analyses of beam profiles for different masses after scattering by a buffer gas permit determination of mixed cluster presence and, if any, of cluster sizes and compositions. The two techniques are applied to supersonic expansions of an argon-nitrogen mixture. We discuss the results that provide new insight in binary nucleation processes. Received: 6 October 1997 / Revised: 4 November 1997 / Accepted: 13 November 1997     

Formation of metal-encapsulating Si cage clusters

We report the formation of a series of metal-containing hydrogenated silicon clusters using an ion trap. Mass analyses reveal that many types of transition metal ions M(+) ( M = Hf, Ta, W, Re, Ir, etc.) react with silane (SiH4) to form dehydrogenated MSi( +)(n) cluster ions ( n = 14, 13, 12, 11, 9, respectively) as an end product, indicating that the metal atom is endohedral and stabilizes the Si polyhedral cage. This finding is confirmed by our ab initio calculation that WSi12 is a W-encapsulating Si12 cage cluster, and is very stable owing to both the electronic and the geometrical shell closures.     

Optical properties of mixed clusters: comparative study of Ni/Ag and Pt/Ag clusters

The optical properties of mixed (Ni_0.5Ag_0.5)_n and Pt/Ag clusters are investigated in the size range 2-5 nm. Low Energy Ion Spectroscopy (LEIS) experiments show that the cluster surface is entirely covered by silver atoms for the two systems. The optical spectra of Ni/Ag clusters exhibit a large Surface Plasmon Resonance (SPR), damped and widened when the cluster size decreases, in agreement with a classical model assuming a core-shell geometry and including the reduction of the conduction electron mean-free path in the silver shell. For Pt/Ag clusters, no SPR emerges in the size range 2-5 nm, although it is predicted within a classical model, a pronounced SPR appearing only for clusters larger than 10 nm in diameter.