Interaction of argon clusters with intense VUV-laser radiation: the role of electronic structure in the energy-deposition process

The response of Ar clusters to intense vacuum-ultraviolet pulses is investigated with photoion spec-troscopy. By varying the laser wavelength, the initial excitation was either tuned to absorption bands of surface or bulk atoms of clusters. Multiple ionization is observed, which leads to Coulomb explosion. The efficiency of resonant 2-photon ionization for initial bulk and surface excitation is compared with that of the nonresonant process at different laser intensities. The specific electronic structure of clusters plays almost no role in the explosion dynamics at a peak intensity larger than 1.8 x 10(12) W/cm(2). The inner ionization of atoms for resonant and nonresonant excitation is then saturated and the energy deposition is mainly controlled by the plasma heating rate. Molecular dynamics simulations indicate that standard collisional heating cannot fully account for the strong energy absorption.     

Small rare gas clusters in XUV laser pulses

Semi-classical molecular dynamics simulations of small rare gas clusters in short laser pulses of 100 nm wavelength were performed. For comparison, the cluster response to 800 nm laser pulses was investigated as well. The inner ionization dynamics of multi-electron atoms inside the cluster was treated explicitly. The simulation results underpin the belief that at XUV (extreme ultraviolet) wavelengths collisions play an important role in the energy absorption. The generation of the surprisingly high charge states of Xe atoms inside clusters, as they were observed in a free-electron laser experiment at DESY, Hamburg, Germany by Wabnitz et al. is due to the reduced ionization potential of atoms inside charged clusters, the ionization ignition mechanism, and collisions. PACS 36.40.Gk; 36.40.Vz; 31.15.Gy     

Mechanical effect of van der waals interactions observed in real time in an ultracold Rydberg gas

We present time-resolved spectroscopic measurements of Rydberg-Rydberg interactions between two Rydberg atoms in an ultracold gas, revealing the pair dynamics induced by long-range van der Waals interactions between the atoms. By detuning the excitation laser, a specific pair distribution is prepared. Penning ionization on a microsecond time scale serves as a probe for the pair dynamics under the influence of the attractive long-range forces. Comparison with a Monte Carlo model not only explains all spectroscopic features but also gives quantitative information about the interaction potentials. The results imply that the interaction-induced ionization rate can be influenced by the excitation laser. Surprisingly, interaction-induced ionization is also observed for Rydberg states with purely repulsive interactions.     

The ionization potentials of clustered sodium atoms

Small clusters of sodium atoms have been produced by the isentropic flow of high pressure vapour through a small orifice. These clusters have been ionized by ultra-violet light and detected using a mass spectrometer. Clusters of up to eight sodium atoms have been observed and their ionization potentials have been measured. The ionization potentials of Na₃ and Na_s are 3.9 v and 4.0 v respectively, showing that even the smallest clusters tend to the value expected for a continuous drop of metal of the same size.     

Density functional investigation of structural and electronic properties of small bimetallic silver–gold clusters

Structural and electronic properties of bimetallic silver–gold clusters up to eight atoms are investigated by the density functional theory using Wu and Cohen generalized gradient approximation functional. By substitution of Ag and Au atoms, in the optimized lowest energy structures of pure gold and silver clusters, we determine the ground state conformations of the bimetallic silver–gold ones. We reveal that Ag atoms prefer internal positions whereas Au atoms prefer exposed ones favoring charge transfer from Ag to Au atoms. For each size and composition, binding energy, HOMO–LUMO gap, magnetic moment, vertical ionization potential, electron affinity and chemical hardness were calculated. On increasing the size of the cluster by varying number of Ag atoms with fixed number of Au ones, vertical ionization potential and electron affinity show obvious odd–even oscillations consistent with the pure Ag and Au clusters. Au atoms inclusion in the cluster increases the binding energy and vertical ionization potential, indicating higher stability as the number of Au atoms grows. The variation of chemical hardness with the composition in a cluster with the same size shows peaks when the number of Ag atoms is greater than or equal to Au ones, corresponding to transition from planar to tri-dimensional structures. For clusters with even number of atoms, the peaks indicate that the clusters with the same number of Ag and Au atoms are the most stable ones. Analyzing the density of states, we found that increasing the concentration of Ag atoms affects the energy separation between the HOMO and the low lying occupied states.     

70S超冷Cs Rydberg原子的动力学演化

利用双光子激发超冷原子获得70S超冷Cs Rydberg原子, 采用脉冲场电离法使Rydberg原子电离, 并用微通道板测量Rydberg原子的信号. 改变激发光和电离电场脉冲的延迟时间和激发光脉冲的宽度, 研究70S超冷Cs Rydberg原子之间的相互作用和动力学演化过程. 利用黑体辐射导致的态转移和相互作用碰撞电离解释了实验结果,实验结果和理论相一致.     

Electron delocalization in magnesium clusters grown in supercold helium droplets

The formation of bare clusters from highly reactive metals can be achieved very effectively by the pickup of atoms into superfluid helium droplets. We report on the experimental observation of electronic shells in small magnesium clusters produced by this method. Mass spectra taken under various ionization conditions show steps and outstanding peaks, as well as pronounced minima. The abundance distribution suggests a transition to full electron delocalization which is complete at about 20 atoms. A so-far-not-reported electron reorganization is observed, leading to a novel shell structure.     

钇小团簇的结构和电离势的计算

采用密度泛函DFT中的B3LYP方法，选择LANL2DZ双ζ基组，优化并得到了Y_n=(n=2—8)小团簇的基态平衡结构，同时计算出其电离势.结果表明，钇原子之间形成团簇最稳定的结构是倾向于平均配位数最大，其电离势没有“奇-偶”振荡或“幻数”效应，表明Y_n团簇光致电离开始主要发生在Y原子局域化的4d轨道上的电子而不是在5s上.对Tomasz提出的钇团簇电离势的解析式进行合理地修正，修正后电离势解析式的计算值与实验值更接近. 关键词： Y团簇 密度泛函 平衡几何结构 电离势     

Highly selective multistep ionization of atoms by laser radiation

The possibility of dramatic selectivity increase during the stepwise ionization of atoms due to selective excitation at every step has been examined. Evaluations have been made to estimate the selectivity of excitation and ionization by laser radiation of some atoms, their isotopic shifts of absorption lines being observed at several excitation steps, for instance those of U, Yb, Gd. During three-step ionization of Yb atoms in atomic beam one may obtain an excitation selectivity equal to 4.4 × 10¹⁶ cm².     

Phase transitions in simple clusters

Formation of the liquid state of clusters with pairwise interactions between atoms is examined within the framework of the void model, in which configurational excitation of atoms results from formation of voids. Void parameters are found from computer simulation by molecular dynamics methods for Lennard-Jones clusters. From that standpoint, phase transitions are analyzed in terms of two aggregate states. This information allows us to divide the entropy jump during a solid-liquid phase transition into two parts: one corresponds to configurational excitation at zero temperature and the other arises from thermal vibrations of atoms. The latter part contributes approximately 40% for Lennard-Jones clusters consisting of 13 and 55 atoms, increasing to 56% for bulk inert gases. These magnitudes explain the validity of melting criteria based on thermal motion of atoms, even though the distinctive mechanism of this phase transition results from configurational excitations. It is shown that the void concept allows analyzing various aspects of the liquid state of clusters including the existence of a limiting freezing temperature below which no metastable liquid state exists, as well as the existence and properties of glassy states that may exist below the freezing limit.     

Solid state nuclear track detectors: Track forming,stabilizing and development processes

Fast moving heavy charged particles passing through solids are mainly losing their energy—in a wide range of velocities—by excitation and ionization processes which result in a more or less stable radiation damage.¹ The radiation damage may consist of broken bonds, free radicals, chemical reaction products, displaced atoms, ionic and electronic defects, dislocation configurations, voids, clusters of defects with and without impurities, nuclei of new phases etc. The nature and stability of this localized radiation damage, termed the “latent” track of the particle depends on the data of the particle and on the physical and chemical properties of the solid. Dielectric materials with low electric and thermal conductivities offer favorable conditions for relatively high local excitation and ionization densities resulting in physical and chemical solid state reactions with relatively stable reaction Products.     

Triple coincidence (e,gamma2e) experiment for simultaneous electron impact ionization excitation of helium

Simultaneous ionization and excitation of helium atoms by 500 eV electron impact is observed by a triple coincidence of an ionized slow electron, the recoiling He+ ion, and the radiated vacuum ultraviolet photon (lambda< or =30.4 nm). Kinematically complete differential cross sections are presented for the He+(2p)2P final ionic state, demonstrating the feasibility of a quantum mechanically complete experiment. The experimental data are compared to predictions from state-of-the-art numerical calculations. For large momentum transfers, a first-order treatment of the projectile-target interaction can reproduce the experimental angular dependence, but a second-order treatment is required to obtain consistent magnitudes.     

The geometry structures and electronic properties of Li_mB_n(m+n=12) clusters

The geometric structures, electronic properties, total and binding energies, harmonic frequencies, the highest occupied molecular orbital to the lowest unoccupied molecular orbital energy gaps, and the vertical ionization potential energies of small LimBn （m＋ n = 12） clusters were investigated by the density functional theory B3LYP with a 6-31 I＋G （2d, 2p） basis set. All the calculations were performed using the Gaussian09 program. For the study of the LimBn clusters, the global minimum of the B 12 cluster was chosen as the starting point and the boron atoms were gradually replaced by Li atoms. The results showed that as the number of Li atoms increased, the stability of the LimBn cluster decreased and the physical and chemical properties became more active. In addition, on average there was a large charge transfer from the Li atoms to the B atoms.     

碱金属原子的光激发与光电离

本文研究了碱金属原子在三步激光脉冲作用下的光激发和光电离过程的动力学特性, 重点关注和比较了锂和铯原子的异同. 针对多种激发模式, 本文不但建立了其原子布居数在各个跃迁态的速率方程组, 还给出了各相关态的光激发和光电离过程的解析解. 通过精心设计并选择了特殊情况, 显著简化了解析解的数学表达式, 从而凸显和讨论了其物理内涵. 通过自行编程, 系统地计算和观察了各种激发模式对锂原子的光激发和光电离过程的可能影响, 研究和讨论了电离率随激光参数的变化规律. 在相同激发模式下, 比较和分析了采用两种不同激发路径所导致的各态原子布居率的变化, 凸显了改变原子参数所产生的作用. 探讨了锂和铯原子在类似的激发条件下在电离率方面的差别. 最后, 基于本文的研究结果, 本文指出了优化电离率的多种途径.     

Resonance ionization spectroscopy of thorium

Here we describe experiments aimed at developing an element-selective ion source for thorium (Th). The technique applied is resonance ionization spectroscopy (RIS) with a thermal atom beam. Ionization schemes for isotopically nonselective ionization of Th as well as for isotopically selective ionization of ²³⁰Th are proposed. The RIS-scheme used is two-photon two-colour ionization with excitation in the ultraviolet spectral range between 244 nm and 267 nm or in the visible spectral range between 485 nm and 529 nm. Ionization of the excited atoms is performed either by ultraviolet photons or by visible photons, depending on the energy required for this process.     

Resonance Ionization Mass Spectrometry (RIMS) with Pulsed and CW-Lasers on Plutonium

The detection of long-lived plutonium isotopes in ultra-trace amounts by resonance ionization mass spectrometry (RIMS) is a well-established routine method. Detection limits of 10⁶ to 10⁷ atoms and precise measurements of the isotopic composition have been achieved. In this work multi-step resonance ionization of plutonium atoms has been performed with tunable lasers having very different output intensities and spectral properties. In order to compare different ways for the resonance ionization of plutonium broadband pulsed dye and titanium:sapphire lasers as well as narrow-band cw-diode and titanium:sapphire lasers have been applied for a number of efficient excitation schemes. It has been shown, that for identical excitation schemes the optical isotope selectivity can be improved by using cw-lasers (bandwidths < 10 MHz) instead of pulsed lasers (bandwidths > 2 GHz). Pulsed and cw-laser systems have been used simultaneously for resonance ionization enabling direct comparisons of pulsed and continuous ionization processes. So far, a three-step, three-color laser excitation scheme has been proven to be most practical in terms of efficiency, selectivity and laser wavelengths. Alternatively a newly discovered three-step, two-color excitation scheme which includes a strong two-photon transition from an excited state into a high-lying autoionizing state yields similar ionization efficiencies. This two-photon transition was characterized with respect to saturation behavior and line width.     

Excitations in charge-transfer atom scattering

The electronic excitations are calculated for a tight-binding model of 25–1000 eV Na atoms scattering off W, assuming a classical trajectory for the Na atoms which interact with a single half-filled band on the substrate. The excitation spectrum consists of substrate electron-hole pairs at low energies, with a jump at the ionization threshold due to electron transfer from the Na to the W. If the Na ionization level crosses the Fermi energy beyond the range of hopping between the Na and the W substrate, the ionization probability is high. As the Na kinetic energy is reduced the ionization probability decreases, but the substrate electron-hole excitations increase in importance, and this is discussed in semi-classical terms.     

Emission of charged clusters during metal sputtering by ions

A method for simulating processes of metal sputtering by ion bombardment in the form of large neutral and charged clusters with a number of atoms N≥5 based on simple physical assumptions and in fair agreement with experiment is suggested. As an example, the ionization degrees and ionization coefficients, as well as the relative cluster yields, are calculated as a function of the number of atoms in clusters of different metals (Ag, Nb, and Ta) bombarded by singly charged Ar⁺¹ and Au⁻¹ ions. A fluctuation mechanism of charge state formation for large clusters, which describes the dependence of the charge state distributions on cluster size and target temperature, is developed.     

ATI of complex systems: Ar and C<Subscript>60</Subscript>

Above threshold ionization of two structurally different systems is presented namely a rare gas such as argon and the more complex C₆₀ fullerene. We show that the ionization dynamics is different and is dominated by the presence of high-lying Rydberg states in Ar and low-lying bound states in C₆₀. The study is based on a theoretical (solving the time dependent Schrödinger equation) and/or experimental (using measurements from a photoelectron imaging spectrometer) aspect.Received: 20 December 2002, Published online: 24 April 2003PACS: 33.80.Rv Multiphoton ionization and excitation to highly excited states (e.g., Rydberg states) - 32.80.Fb Photoionization of atoms and ions - 36.40.-c Atomic and molecular clusters - 33.60.-q Photoelectron spectra - 61.48.+c Fullerenes and fullerene-related materials