The new ClusterTrap setup

ClusterTrap has been designed to investigate properties of atomic clusters in the gas phase with particular emphasis on the dependence on the cluster size and charge state. The combination of cluster source, Penning trap and time-of-flight mass spectrometry allows a variety of experimental schemes including collision-induced dissociation, photo-dissociation, further ionization by electron impact, and electron attachment. Due to the storage capability of the trap extended-delay reaction experiments can be performed. Several recent modifications have resulted in an improved setup. In particular, an electrostatic quadrupole deflector allows the coupling of several sources or detectors to the Penning trap. Furthermore, a linear radio-frequency quadrupole trap has been added for accumulation and ion bunching and by switching the potential of a drift tube the kinetic energy of the cluster ions can be adjusted on their way towards or from the Penning trap. Recently, experiments on multiply negatively charged clusters have been resumed.     

Multiply charged titanium cluster anions: production and photodetachment

Titanium clusters are produced by laser vaporization of a metal wire in a helium gas pulse, stored in a Penning trap, size selected and transformed into multiply charged anions by electron attachment. Both doubly and triply charged titanium clusters are observed. For the first observation of photodetachment of electrons from metal cluster dianions, Ti ₅₅ ^2- clusters are selected and excited by a laser pulse, which leads to the emission of an excess electron: Ti ₅₅ ^2- → e⁻ + Ti ₅₅ ^- . This revised version was published online in August 2006 with corrections to the Cover Date.     

On the decay of hot metallic clusters by evaporation

Starting from the Weisskopf theory decay rates for the evaporation of cluster atoms from hot liquid alkali metal clusters are derived. The crucial input quantity is the level density which is determined from empirical properties of the bulk, namely from the specific heat and the thermal expansion coefficient. The resulting rate expression is compared with decay rate formulas given by Engelking, Klots and Gspann. Furthermore, critical (appearance) sizes of multiply charged clusters are calculated by equating the rates for neutral monomer and light charged particle emission. Also shrinking and cooling rates of large hot clusters are determined by treating multiple emission of cluster atoms, thus establishing a time scale for the decay of clusters theoretically.     

Rayleigh instabilities in multiply charged sodium clusters

The stability of multiply charged sodium clusters Na(q+)(n) (q< or =10) produced in collisions between neutral clusters and multiply charged ions A(z+) ( z = 1 to 28) is experimentally investigated. Multiply charged clusters are formed within a large range of temperatures and fissilities. They are identified by means of a high-resolution reflectron-type time-of-flight mass spectrometer (m/deltam approximately 14 000). The maximum fissility of stable clusters is obtained for z = 28 and is X approximately 0.85+/-0.07, slightly below the Rayleigh limit (X = 1). It is mainly limited by the initial cluster temperature (T approximately 100 K).     

Recombination processes in atomic clusters irradiated by superintense femtosecond laser pulses

Various mechanisms of recombination of electrons with multiply charged atomic ions in atomic clusters irradiated by superintense femtosecond laser pulses are discussed. All of the recombination mechanisms are shown to take a time considerably longer than the laser pulse duration and, hence, they can develop only in a homogeneous, fairly rarefied cluster plasma after pulse termination. All autoionization states of multiply charged ions in a dense cluster plasma have been found to be destroyed by the Holtsmark electric field.     

中等光强纳秒激光电离苯团簇产生多价碳离子的数值模拟和实验研究

飞秒强激光与团簇相互作用产生多价离子的现象已被广泛报道,然而近期多个研究小组发现当功率密度低至1010W/cm2的纳秒激光照射团簇时,同样也观察到了多价离子的存在.虽然可以用"多光子电离引发-逆韧致吸收加热-电子碰撞电离"电离机理对这种现象进行解释,但是缺乏相应的数值模拟.建立了一个简化的数值模型,根据有质动力势Up计算团簇内电子能量,再由Lotz公式计算出相应的电离截面,最后由动力学反应速率方程计算出团簇内多价碳离子随时间的演变.详细分析了团簇尺寸、电子密度等关键参数对多价离子产生的影响.数值模拟结果表明:团簇电离在小于0.7 ns时间尺度内完成,C2+,C3+和C4+多价离子强度达到平衡后,离子相对强度由大到小依次为C2+,C3+,C4+,这与实验结果相一致;多价离子的价态随着团簇尺寸的增加而升高,半径为5.6 nm的苯团簇比半径为3 nm的苯团簇更容易产生高价态的离子,这也与实验结果相一致.     

Charge localization in collision-induced multiple ionization of van der Waals clusters with highly charged ions

Charge localization in multiple ionization and fragmentation of small argon clusters is reported. The processes are initiated by interaction of the neutral cluster with highly charged Xe(q+) (5< or =q< or =25). Products are detected by means of multicoincidence time-of-flight methods. A strong dependence of the fragmentation pattern on the Xe charge state q is observed. In particular, we find evidence for formation of multiply charged atomic Ar(r+) fragment ions up to r = 7. Such high charge states have neither been observed in fission of multiply charged van der Waals clusters nor in ion-induced fragmentation of fullerenes or metal clusters. This hints at fundamentally different excitation and fragmentation dynamics.     

Observation of persistent flow of a Bose-Einstein condensate in a toroidal trap

We have observed the persistent flow of Bose-condensed atoms in a toroidal trap. The flow persists without decay for up to 10 s, limited only by experimental factors such as drift and trap lifetime. The quantized rotation was initiated by transferring one unit variant Planck's over 2pi of the orbital angular momentum from Laguerre-Gaussian photons to each atom. Stable flow was only possible when the trap was multiply connected, and was observed with a Bose-Einstein condensate fraction as small as 20%. We also created flow with two units of angular momentum and observed its splitting into two singly charged vortices when the trap geometry was changed from multiply to simply connected.     

The SMILETRAP (Stockholm-Mainz-Ion-LEvitation-TRAP) facility

Described in this paper is an experimental facility which measures atomic masses by using multiply charged ions from an electron beam ion source. The ions are injected into a Penning trap and the cyclotron frequencies measured. A precision of 2×10^–9 has been reached using highly charged carbon, nitrogen, oxygen and neon.     

On the fragmentation of multiply charged sodium clusters

The fragmentation of multiply charged atomic sodium clusters of mass 200 is investigated using the Micro-canonical Metropolis Monte Carlo (MMMC) statistical technique for excitation energies up to 200 eV and for cluster charges up to +9e. In this work we present caloric curves and charged and uncharged fragment mass distributions for clusters with charges 0, 2, and 4. The caloric curves show a dip at the critical point implying a negative specific heat, as expected for finite systems, while the fragment mass distributions corroborate the picture of a phase transition from one dominant liquid-like cluster to complete vaporization. Received 7 November 2001 / Received in final form 4 April 2002 Published online 28 June 2002     

MIS-1 electron-beam ion source

The Institute of Nuclear Physics (INP) has developed and produced electron-beam multiply charged ion sources. These ion sources give the electron beam its high density in the ionization area, at the ion trap ≥10³ A/cm². They produce multiply charged ions of various elements, both gaseous and solid ones. These ion sources successfully employ the technique of the dozed inlet of solid-element atoms into the ion trap.     

Dissociation pathways of doubly and triply charged gold clusters

Collision induced dissociation is applied to study the fragmentation channels of multiply charged gold clusters, Au N2⁺, size N= 7 –35, and Au> _N3+}, N = 19–35, stored in an ion cyclotron resonance (Penning) trap. The main dissociation pathways are neutral monomer evaporation, Au> _NZ+to Au> _N-1Z+} + Au, for the larger and fission into a charged trimer plus the remaining cluster, Au> _NZ+to{}Au> _N-3(Z-1)+} +{}Au> ₃₊}, for the smaller clusters. In the intermediate cluster size region an odd–even alternation of the two competing decay pathways is observed. In addition, for some specific cluster sizes there are indications of neutral dimer evaporation, Au> _NZ+to{}Au> _N-2Z++Au> ₂}, and of extremely asymmetric fission of the form Au> _NZ+to Au> _N-1(Z-1)+} + Au⁺. This revised version was published online in July 2006 with corrections to the Cover Date.     

Stability and fragmentation processes of highly charged sodium clusters

Highly charged sodium clusters produced in collisions between neutral clusters and multiply charged ions are formed within a large range of temperatures and fissilities, and identified by means of a high-resolution reflectron-type time-of-flight mass spectrometer ( m/m 14000). The limit of stability of these charged clusters is experimentally investigated, and the time-of-flight spectra are compared with theoretical spectra based on Monte-Carlo simulations. The results indicate that the maximum fissility (X) of stable clusters is approaching the Rayleigh limit (X = 1) for larger clusters sizes. It is mainly limited by the initial neutral cluster temperature ( T 100 K) and the energy transfer in the ionizing collision. In addition, the comparison between the measured and simulated spectra suggests for high cluster charges a multi-fragmentation process, in which most of charge is emitted, creating low charged residual cluster ions.     

Experiments on clusters

In this contribution we discuss four different types of experiments that have been conducted at molecular beams of neutral clusters. The size of particularly stable sodium chloride clusters and their corresponding geometrical structure is inferred from intensity anomalies in mass spectra. This information is obtained either for charged or for neutral clusters depending on whether the clusters are ionized by electron impact or by multiphoton absorption. The important role of fragmentation in mass spectrometry of xenon clusters is revealed by multiphoton ionization; dissociative reactions occurring on the time scale of 10⁻⁷ s with respect to the ionizing event can be analyzed. The solvation energy of negatively charged carbon dioxide clusters as a function of cluster size is obtained from electron attachment spectra. A resonance in the ion yield close to zero eV electron energy signifies that all clusters except for the monomer feature a positive electron affinity. An analysis of the kinetic energy of fragment ions, originating from delayed dissociation of triply charged carbon dioxide clusters, reveals that the size distribution of their fission fragments is extremely symmetric.     

Generation of a high-current beam of multiply charged ions from a dense plasma produced by high-power millimeter-wave gyrotron radiation under ECR conditions

Experimental data for generating intense beams of multiply charged heavy gas ions are reported. The beams are extracted from the dense plasma of an ECR discharge with quasi-gasdynamic confinement provided by the powerful microwave radiation of a gyrotron in a magnetic trap. The axisymmetric magnetic trap makes it possible to extract uniform (in transverse coordinates) plasma fluxes from it, and the use of a multiple-aperture extraction system makes it possible to increase the beam current by more than an order of magnitude compared with the ECP sources currently available. Multiply charged nitrogen ion beams with a current of 150 mA and a normalized emittance of 0.9π mm mrad are obtained.     

电离效率对激光电离团簇的高价离子产物的影响

纳秒激光与团簇相互作用产生高价离子逐渐成为分子物理界的热点之一, 为了深入研究团簇电离的本质, 本文以分子结构相似、元素组成相同的苯、环己烯和环己烷的分子团簇为对象, 利用飞行时间质谱研究了其与5 ns的532 nm激光相互作用时电离产物的价态和强度分布. 结果表明: 这三种化合物多光子电离效率苯>环己烯>环己烷, 但其高价离子的价态和比值苯是最低的, 环己烷的碳离子最高价态为4价, C³⁺和C²⁺的比值为1.1; 环己烯电离产物C³⁺和C²⁺ 的比值降低为0.6; 苯团簇的最高价态只有3价, C³⁺和C²⁺的比值约为0.4. 引起这种现象的原因可以归结于高的多光子电离效率会导致团簇多位点的电离, 引起团簇在电子加热到发生碰撞电离之前发生解离, 减小了团簇的尺寸, 进而减少了离子发生碰撞电离产生高价离子的反应时间, 最终阻碍了高价态离子的产生.     

Multiply charged neon clusters: failure of the liquid drop model?

We have analyzed the stability and fission dynamics of multiply charged neon cluster ions. The critical sizes for the observation of long-lived ions are n2=284 and n3=656 for charge states 2 and 3, respectively, a factor 3 to 4 below the predictions of a previously successful liquid-drop model. The preferred fragment ions of fission reactions are surprisingly small (2相似文献   

Electron binding energies from collisional activation of metal-cluster dianions

Gold-cluster dianions $\mathrm{Au}_{n}^{2-}$ , n=21–31, have been investigated by use of multi-collisional excitation in a Penning trap. At low excitation energies the corresponding singly charged cluster anions have been observed, but no fragments, which indicates the emission of one electron. The binding energy of the surplus electron is deduced from the dianion yield observed as a function of the collision energy by use of a statistical model based on detailed balance. The resulting binding energies of the second electrons are in good agreement with a simple liquid-drop model with empirical corrections including the Coulomb barrier. The double difference of these energies shows a strong odd–even staggering which is compared to the behavior of the electron affinity of neutral gold clusters.     

Observation of multiply charged silver-cluster anions

Singly charged silver-cluster anions are produced in a laser vaporization source and transferred into a Penning trap. After size selection the clusters are subjected to an electron bath in the trap, which results in the attachment of further electrons. The relative abundance of dianions or trianions as a function of the clusters' size is analyzed by time-of-flight mass spectrometry. Silver-cluster dianions are observed for sizes n≥ 24 and trianions for n > 100. In addition, a detailed study of the cluster sizes 24 ?n? 60 shows a pronounced resistance to electron attachment for singly charged anions Ag_n ^- with a closed electronic shell, in particular Ag₂₉ ^-, Ag₃₃ ^-, and Ag₃₉ ^-. Both the threshold size for the observation of dianionic silver clusters and the shell effects in the production yield correlate favorably with previous theoretical investigations of the respective electron affinities. Received 24 November 2000     

Ellipticity-dependent of multiple ionisation methyl iodide cluster using 532 nm nanosecond laser

The dependence of multiply charged ions on laser ellipticity in methyl iodide clusters with 532 nm nanosecond laser was measured using a time-of-flight mass spectrometer. The intensities of multiply charged ions I^q+(q = 2–4) with circularly polarised laser pulse were clearly higher than those with linearly polarised laser pulse but the intensity of single charged ions I⁺ was inverse. And the dependences of ions on the optical polarisation state were investigated and a flower petal and square distribution for single charged ions (I⁺, C⁺) and multiply charged ions (I²⁺, I³⁺, I⁴⁺, C²⁺) were observed, respectively. A theoretical calculation was also proposed to simulate the distributions of ions and theoretical results fitted well with the experimental ones. It indicated that the high multiphoton ionisation probability in the initial stage would result in the disintegration of big clusters into small ones and suppress the production of multiply charged ions.