Laser-cluster interaction: x-ray production by short laser pulses

We investigate the heating of the quasifree electrons in large rare-gas clusters (N exceeding 10(5) atoms) by short laser pulses at moderate intensities (I approximately = 10(15) W cm(-2)). We identify elastic large-angle backscattering of electrons at ionic cores in the presence of a laser field as an efficient heating mechanism. Its efficiency as well as the effect of collective electron motion, electron-impact ionization, and cluster charging are studied employing a mean-field classical transport simulation. Results for the absolute x-ray yields are in surprisingly good quantitative agreement with recent experimental results.     

Ionization of clusters in strong x-ray laser pulses

The effect of intense x-ray laser interaction on argon clusters is studied theoretically with a mixed quantum/classical approach. In comparison to a single atom we find that ionization of the cluster is suppressed, which is in striking contrast to the observed behavior of rare-gas clusters in intense optical laser pulses. We have identified two effects responsible for this phenomenon: A high space charge of the cluster in combination with a small quiver amplitude and delocalization of electrons in the cluster. We elucidate their impact for different field strengths and cluster sizes.     

Self-action of laser radiation in cluster plasma

We have analytically and numerically studied the self-action dynamics of laser radiation in a plasma with ionized gas clusters. Based on the simplified model of a cluster in the form of a superposition of two charged (electron and ion) bunches, we analyze the nonlinearity mechanisms. We refine the electrodynamic cluster model by the molecular dynamics method. The polarization behavior of the plasma bunch in the main part of the laser pulse is shown to be the same as that in the simplified model. We investigate the self-action dynamics of laser radiation under conditions when the nonlinearity of the stratified medium is determined by the anharmonicity of the electron motion in the cluster, while the group velocity dispersion is determined by both the background plasma and the ionized clusters. Since the characteristic field for the electron nonlinearity depends strongly on the cluster size, the peculiarities of the self-action dynamics result from plasma bunch expansion. The spatiotemporal evolution of the wave field is shown to be accompanied by pulse self-compression near the trailing edge.     

Velocity dependence of metal cluster deposition on an insulating surface

We present a detailed study of the deposition of small sodium clusters on a NaCl surface. To that end, we use a microscopic model based on the Time-Dependent Local Density Approximation (TDLDA) for electrons, coupled to classical Molecular Dynamics (MD) for ions. We discuss in particular the deposition mechanism for different initial cluster velocities and demonstrate that extremely slow velocities are necessary to ensure a cluster deposition without damaging the original cluster.Received: 13 March 2004, Published online: 11 May 2004PACS: 36.40.Cg Electronic and magnetic properties of clusters - 36.40.Sx Diffusion and dynamics of clusters - 68.49.Fg Cluster scattering from surfaces     

气相过渡金属钽碳链团簇的研究

Nd:YAG产生的二倍频532nm激光消融金属靶表面,同时含有3%乙炔的氦载气喷向旋转的金属靶,通过等离子体反应形成中性的气相碳链-金属团簇分子。然后经过超声膨胀后,由skimmer形成准直的分子束,进入飞行时间质谱仪的电离区,被电离激光电离。当电离激光波长为248nm时,只观察到了TaCy+（y = 0-10）的碳链团簇离子信号,实验发现奇数碳链的过渡金属钽团簇离子信号比较小,而偶数碳链的团簇离子信号较大。当电离激光波长为266nm时,观察到了TaxCy+（x = 1-4,y = 0-4）的碳链团簇离子信号。     

Plasmon-enhanced electron acceleration in intense laser metal-cluster interactions

We have measured the energy and angular-resolved electron emission from medium-sized silver clusters (N approximately 500-2000) exposed to dual laser pulses of moderate intensity (I approximately (10(13-14) W/cm2). When the second pulse excites the plasmon resonantly, we observe enhanced emission along the laser polarization axis. The asymmetry of the electron spectrum is strongly increasing with electron energy. Semiclassical simulations reveal the following mechanism: Electrons bound in highly excited states can leave, return to, and traverse the cluster. Those electrons that return at zero plasmon deflection and traverse the cluster during a favorable plasmon half-cycle can experience maximum acceleration by the evolving polarization field. As a result of these constraints energetic electrons are emitted in direction of the laser polarization axis in subcycle bursts.     

Ionization dynamics of simple metal clusters in intense fields by the Thomas-Fermi-Vlasov method

The time-dependent response of simple metal clusters to femtosecond laser pulses is investigated using the semiclassical theory based on the Vlasov equation. Starting from a Thomas-Fermi ground state the dynamics are calculated by use of the pseudoparticle method. Systems studied here are sodium clusters containing up to 147 atoms. Both, the energy transfer to the cluster, which is largely affected by the plasmon enhanced absorption, and the following release of energy to the ions are examined in detail. During the laser excitation the feedback of the absorption to the development of the plasmon energy is controlled by competing mechanisms: ionization and cluster expansion. Characteristics of the Coulomb explosion are studied as function of photon energy and cluster size, particularly with regard to the dynamical influence of collective excitations of the electrons. We also predict features in the angular distribution of the ions that could be measured to test the calculated dynamics.Received: 9 December 2003, Published online: 16 March 2004PACS: 52.50.Jm Plasma production and heating by laser beams (laser-foil, laser-cluster, etc.) - 36.40.Vz Optical properties of clusters - 36.40.Gk Plasma and collective effects in clusters     

Mechanisms for second harmonic generation in the interaction of a superintense ultrashort laser pulse with cluster plasma

The effects of the interaction of an intense femtosecond laser pulse with large atomic clusters are considered. The pulse intensity is of the order of 10¹⁸ W cm^?2. New effects appear when the magnetic component of the Lorentz force is taken into account. The second harmonic of laser radiation is generated. The second harmonic generation (SHG) efficiency is proportional to the square of the number of atoms in a cluster and the square of the laser radiation intensity. The resonance increase in the SHG efficiency at the Mie frequencies (both at the second harmonic frequency and fundamental frequency) proved to be insignificant because of the fast passage through the resonance during cluster expansion. The mechanisms of the expansion and accumulation of energy by electrons and ions in the cluster are discussed in detail. The energy accumulation by electrons mainly occurs due to stimulated inverse bremsstrahlung upon elastic reflection of the electrons from the cluster surface. The equations describing the cluster expansion take into account both the hydrodynamic pressure of heated electrons and the Coulomb explosion of the ionized cluster caused by outer shell ionization. It is assumed that both inner shell and outer shell ionization is described by the over barrier mechanism. It is shown that atomic clusters are more attractive for the generation of even harmonics than compared to solid and gas targets.     

Small rare-gas clusters in soft x-ray pulses

We develop a microscopic model for the interaction of small rare-gas clusters with soft x-ray radiation from a free electron laser. It is shown that, while the overall charging of the clusters is rather low, unexpectedly high atomic charge states can arise due to charge imbalances inside the cluster. These findings are explained by an increased absorption via inverse bremsstrahlung due to high intermediate charge states and by a nonhomogenous charge distribution inside the cluster.     

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.     

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.     

Dynamic polarization in the strong-field ionization of small metal clusters

We report on the strong field ionization of small transition metal clusters (nickel, Ni(n) n=1-36) within the quasistatic regime at an infrared wavelength of 1.5 microm and at intensities up to 2 x 10(14) W/cm(2). From ion yields in a constant axial intensity beam, we obtained saturation intensities for the individual Ni(n) clusters. As compared to quasistatic, single active electron calculations, a dramatic suppression of ionization was observed. Dynamic polarization in the laser field likely leads to strong multielectron screening of the "active" electron. Representing the metal clusters as classical conducting spheres, we obtained, via a barrier suppression calculation, the classical ionization rates. Agreement was obtained for larger clusters with n>10 when the dynamic polarization was taken into account, emphasizing the multielectron nature of the ionization suppression.     

Selecting molecules embedded in nanodroplets (clusters) of superfluid helium

A method of selecting molecules embedded in nanodroplets (clusters) of superfluid helium is proposed, which is based on the selective vibrational excitation of embedded molecules by intense IR laser radiation. This action leads to a significant decrease in size of the excited clusters, after which these clusters are separated with respect to size via scattering of the cluster beam on a crossing atomic beam. The method is described in detail and the possibility of selecting SF₆ molecules in liquid helium nanodroplets using the excitation by CO₂ laser radiation and the angular separation via scattering on a xenon atomic beam is demonstrated. The results show that, by using this technique, it is possible to separate molecules with respect to isotope (element) composition. Advantages and drawbacks of the method are analyzed.     

Propagation of the high power laser pulse in multicomponent cluster targets

We present the results of 3D PIC and 2D PIC simulations of the ultra short high irradiance laser pulse interaction with targets where the plasma containing multicomponent cluster targets and multicluster cloud is imbedded in an underdense plasma. In both cases the laser radiation expels the electrons from the clusters and ejects them into the wake plasma wave generated by the ultrashort laser pulse in the underdense plasma. This provides a novel mechanism for the electron injection into the wake field for acceleration.     

MEASUREMENT OF IONIC ENERGY FROM FEMTOSECOND LASER-HEATED ARGON CLUSTERS

The high backing pressure argon gases adiabatically expand into vacuum through a pulsed gas jet to nucleate into large clusters. The clusters were heated by a 45fs, 2.3×10¹⁶ Wcm^-2 Ti: sapphire laser. The high energy of the ions produced in the cluster explosion was measured using time-of-flight spectrometry. The maximum and average kinetic energy of the ions were 0.2MeV and ～12.5keV, respectively, indicating that the femtosecond laser interactions with argon clusters are more energetic than interactions with atoms and molecules.     

甲醇/水混合团簇的多光子电离质谱研究

利用多光子电离技术结合飞行时间质谱仪对甲醇/水混合团簇进行了研究.在脉冲激光波长为355 nm条件下观测到团簇离子.主要的电离产物为质子化的(CH3OH)n(H2O)H+(n=l-13)混合团簇离子与(CH3OH)nH+团簇离子,经分析(CH3OH)1o(H2O) H+和(CH3OH)3H+为幻数结构.甲醇水混合团簇电离后团簇离子发生内部质子化转移反应是形成质子化团簇离子的主要原因.不同尺寸团簇离子信号强度随电离激光光强变化的光强指数曲线显示,团簇均发生四光子电离过程.     

Guiding of intense laser pulses in plasma waveguides produced from efficient, femtosecond end-pumped heating of clustered gases

We demonstrate intense pulse guiding in efficient femtosecond end-pumped waveguides generated in clustered gases. This novel scheme provides a route to significantly lower on-axis plasma density (< 10(18) cm(-3)) more than is feasible in conventional hydrodynamic plasma waveguides. Self-focused propagation and strong absorption of intense femtosecond laser pulses are used to produce long centimeter scale channels in an argon cluster jet, and a subsequent pulse is guided with 3 x 10(17) W cm(-2) intensity and approximately 50% coupling efficiency. Preliminary results with hydrogen clusters also show guiding.