Charging dynamics of metal clusters in intense laser fields

Clusters of heavy metal atoms in strong femtosecond laser-light fields undergo multi-ionization with the loss of hundreds of electrons. The cross section largely exceeds that of corresponding isolated atoms, which leads in the case of Pb_N to a complete ionization of the 4f shell with a light intensity of 1.2×10¹⁵ W/cm². Experimental investigations on Pb and Pt clusters with variable pulse widths and, for the first time, with the pump&probe technique give insight into the dynamics of the coupling of electromagnetic radiation into the clusters. Both approaches support the picture according to which, after an initial charging, the clusters expand due to Coulomb forces. This expansion is accompanied by a reduction of the electron density and at the same time by an increase of the optical sensitivity. Once the plasmon energy of the diluted nanoplasma approaches the photon energy, the charging efficiency increases significantly. The experimental observations are confirmed by random-phase approximation (RPA) calculations of the optical response, including molecular-dynamics simulations of the expanding systems. Received: 11 November 1999 / Published online: 13 July 2000     

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     

Xenon clusters in intense VUV laser fields

A simple model is developed that quantitatively describes intense interactions of a vacuum ultraviolet (VUV) laser pulse with a xenon cluster. We find good agreement with a recent experiment [Nature (London) 420, 482 (2002)]]. In particular, the large number of VUV photons absorbed per atom, at intensities significantly below 10(16) W/cm(2), is now understood.     

高频强激光场中H-电离特性理论研究

高频强激光场中高价负离子（比如H-,H2-,He-,He2-等等）的稳定存在虽然在理论上早已得到得到证明,但在实验上至今没有被直接验证。为了探索可行的实验验证方案,通过以高频强场中的负一价氢离子H-为例,采用相空间平均法,详细研究了其在外加激光场中的电离率及光电子角分布情况。研究发现 的电离率比氢原子高,并且不存在氢原子在较强激光场中的电离抑制现象。另外随着激光场强度的增大和激光频率的减小,电子角分布与H-在高频场直接卸载后电子角分布的差别也增大。这些结果为将来在实验上验证高频强场中高价负离子的存在性提供了很好的理论依据。     

Asymmetric high-energy ion emission from argon clusters in intense laser fields

Clusters of 2x10(3) to 4x10(4) Ar atoms are Coulomb exploded in intense (up to 8x10(15) W cm(-2)) laser fields. The dependence of multiply charged argon ion energies on the polarization state of light is probed. A directional asymmetry in the ion-explosion energies is observed for the highest charge states. The ion-energy distribution consists of a low-energy isotropic component, and a high-energy anisotropic one. The results are discussed in terms of an asymmetric Coulomb-explosion scenario.     

Dynamics of free and embedded lead clusters in intense laser fields

Lead clusters are exposed to strong femtosecond light pulses. The dependence of the recoil energy on the charge state of the atomic ion is now investigated using a new detection setup, i.e., a Thomson analyser. First results show that in contrast to laser-induced overdense plasmas at surfaces the recoil energy distribution appears much narrower. Comparing free lead clusters with lead clusters embedded in large helium droplets, the charging dynamics show distinct differences on the femtosecond time scale. In the embedded case the maximum ionization enhancement is reached earlier.     

The effect of volumetric weighting in the interaction of intense laser fields with clusters

Silver clusters embedded in helium nanodroplets are exposed to intense femtosecond laser pulses (10¹³ - 10¹⁶ W/cm²). The signal of highly charged (q≤11) atomic fragments is maximized by delayed plasmon enhanced ionization using stretched laser pulses. Further details with respect to the dynamics of the charging process can be obtained, when the intensity distribution within the laser focus is taken into account. For the first time, the z-scan method is applied to clusters which offers a route to investigate the explicit dependence of the ion signals with respect to the laser intensity. By taking advantage of the volumetric weighting effect ionization thresholds are determined, yielding values well below 10¹⁴ W/cm² for Ag^q+ ions with q≤11.     

Resonant charging of Xe clusters in helium nanodroplets under intense laser fields

We theoretically investigate the impact of multiple plasmon resonances on the charging of Xe clusters embedded in He nanodroplets under intense pump-probe laser excitation (τ = 25 fs, I ₀ = 2.5 × 10¹⁴   W/cm², λ = 800 nm). Our molecular dynamics simulations on Xe₃₀₉He_10 000 and comparison to results for free Xe₃₀₉ give clear evidence for selective resonance heating in the He shell and the Xe cluster, but no corresponding double hump feature in the final Xe charge spectra is found. Though the presence of the He shell substantially increases the maximum charge states, the pump-probe dynamics of the Xe spectra from the embedded system is similar to that of the free species. In strong contrast to that, the predicted electron spectra do show well-separated and pronounced features from highly efficient plasmon assisted electron acceleration for both resonances in the embedded clusters. A detailed analysis of the underlying ionization and recombination dynamics is presented and explains the apparent disaccord between the resonance features in the ion and electron spectra.     

Nanoplasma dynamics in Xe clusters driven by ultraintense laser fields

We present a theoretical and computational study of the properties and the response of the nanoplasma and of outer ionization in Xe_n clusters (n = 55–2171, initial cluster radius R₀ = 8.7–31.0 ?) driven by ultraintense near-infrared laser fields (peak intensity I_M = 10¹⁵–10²⁰ Wcm^-2, temporal pulse length τ= 10–100 fs, and frequency ν= 0.35 fs^-1). The positively charged high-energy nanoplasma produced by inner ionization nearly follows the oscillations of the fs laser pulse and can either be persistent (at lower intensities of I_M = 10¹⁵–10¹⁶ Wcm^-2 and/or for larger cluster sizes, where the electron energy distribution is nearly thermal) or transient (at higher intensities of I_M = 10¹⁸–10²⁰ Wcm^-2 and/or for smaller cluster sizes). The nanoplasma is depleted by outer ionization that was semiquantitatively described by the cluster barrier suppression electrostatic model, which accounts for the cluster size, laser intensity and pulse length dependence of the outer ionization yield. The electrostatic model was further utilized for estimates of the laser intensity and pulse width dependence of the border radius R₀ ^(I) for the attainment of complete outer ionization at , while at R₀ > R₀ ^(I) a persistent nanoplasma prevails. R₀ ^(I) establishes an interrelationship between electron dynamics and nuclear Coulomb explosion dynamics in ultraintense laser-cluster interactions.     

Interaction of intense laser pulses with hydrogen atomic clusters

The interaction between intense femtosecond laser pulses and hydrogen atomic clusters is studied by a simplified Coulomb explosion model. The dependences of average proton kinetic energy on cluster size, pulse duration, laser intensity and wavelength are studied respectively. The calculated results indicate that the irradiation of a femtosecond laser of longer wavelength on hydrogen atomic clusters may be a simple, economical way to produce highly kinetic hydrogen ions. The phenomenon suggests that the irradiation of femtosecond laser of longer wavelength on deuterium atomic clusters may be easier than that of shorter wavelength to drive nuclear fusion reactions. The product of the laser intensity and the squared laser wavelength needed to make proton energy saturated as a function of the squared cluster radius is also investigated. The proton energy distribution calculated is also shown and compared with the experimental data. Our results are in agreement with the experimental results fairly well.     

强激光场中真空极化效应

通过求解狄拉克方程,对强激光场下真空极化问题进行了研究。理论计算结果表明：在仅随时间变化的电场下,要激发狄拉克海中负能级的电子,需要两个阈值条件,即激光场的电场强度大于等于1016 V/cm和激光场的持续时间大于等于10-21 s。前者主要保证负能态电子有足够的能量跃迁到正能态,后者主要是保证电子在跃迁过程中动量亏损得以补偿。     

强激光场中真空极化效应

 通过求解狄拉克方程,对强激光场下真空极化问题进行了研究。理论计算结果表明：在仅随时间变化的电场下,要激发狄拉克海中负能级的电子,需要两个阈值条件,即激光场的电场强度大于等于10¹⁶ V/cm和激光场的持续时间大于等于10^-21 s。前者主要保证负能态电子有足够的能量跃迁到正能态,后者主要是保证电子在跃迁过程中动量亏损得以补偿。     

Nonsequential double recombination in intense laser fields

A second plateau in the harmonic spectra of laser-driven two-electron atoms is observed both in the numerical solution of a low-dimensional model helium atom and using an extended strong field approximation. It is shown that the harmonics well beyond the usual cutoff are due to the simultaneous recombination of the two electrons, which were emitted during different, previous half-cycles. The new cutoff is explained in terms of classical trajectories. Classical predictions and the time-frequency analysis of the ab initio quantum results are in excellent agreement. The mechanism corresponds to the inverse single photon double ionization process in the presence of a (low frequency) laser field.     

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.     

Ionization of atoms and ions by intense laser radiation

The ionization of negative ions by ultrashort electromagnetic pulses, the multiphoton ionization of atoms beyond the perturbation theory taking into account the Coulomb interaction, and the relativistic theory of tunneling in application to the ionization problems have been analyzed. The main results have been obtained using the imaginary time method.