Absolute ionization rates of multielectron transition metal atoms in strong infrared laser fields

We report on nonresonant strong field ionization of the multielectron transition metal atoms V, Nb, Ta, Ni, and Pd. Operating in the adiabatic regime (lambda = 1.5 microm), we quantitatively determined both (i) the first charge state saturation intensities and (ii) the absolute ionization rates for intensities ranging from threshold up to 3 x 10(14) W/cm2. We observed a dramatic suppression of ionization relative to single active electron approximation expectations. We suggest that this derives from dynamic polarization or screening effects within the multielectron atom, stressing a need for many-body theories of strong field ionization.     

Nin(n≤8)团簇的结构

用高斯程序的B3LYP交换相关函数和全电子基组DGDZVP、TZVP优化Ni_n、Ni_n⁺和Ni_n^-(n=2~8),得到这些体系的基态几何构型、离化能、电子亲和能及键能.结果表明:Ni₂,Ni₃,Ni₄,Ni₅和Ni₆团簇的基态分别是5,7,9,11和13重态.表明:Ni₂,Ni₃,Ni₄,Ni₅和Ni₆团簇中分别有4,6,8,10和12个平行自旋的电子,在每一个Ni_n团簇中非耦合的电子最多,这些电子占据不同的轨道,导致每一个Ni_n团簇的能量最小,说明在这些Ni_n团簇中电子平行的效应大于电子耦合的效应,这显然与d电子的离域效应有关,称为自旋极化效应,符合宏特规则.Ni_n、Ni_n⁺和Ni_n^-(n=2~8)体系的磁矩分别是Ni_n具有8μ_B(n=6~8),Ni_n⁺具有9μ_B(n=6~8),Ni_n具有7μ_B(n=4~8).     

Saturated ionization of fullerenes in intense laser fields

We investigate the ionization of icosahedral fullerenes (C20, C60, C80, and C180) in an intense laser pulse using the S-matrix theory. The results obtained are in excellent agreement with the recent observations of unexpectedly high saturation intensities of the Buckminster fullerene and its multiply charged ions. Our analysis strongly suggests that the related phenomenon of suppressed ionization of these complex fullerenes is due to the finite cage size and the "multislit" interference effect between partial waves emitted from the different nuclei rather than to a dynamical multielectron polarization effect.     

超短脉冲强激光场中电子剩余能计算

为了控制光场感应电离等离子体的温度以使得基于光场感应电离机制的X射线激光辐射获得更高的增益值,利用准静态隧道电离模型,定量计算了电子剩余能量与激光偏振参量、波长(频率)、激光强度以及电离介质电离能的变化关系。计算结果表明线偏振短波长激光以及高电离能介质产牛的等离子体中电子剩余能比较低,因此适合用作复合机制X射线激光;对于低价离子存偏振度α介于0～1之间的某一处最高,因此,可以通过调整偏振度α,获得某一椭圆偏振光,会更有利于基于光场感应电离电子碰撞机制X射线激光增益的提高。     

Comparison study of atomic and molecular single ionization in the multiphoton ionization regime

In this Letter, we report, for the first time in the multiphoton ionization regime, a comparison study of single-electron ionization of diatomic molecules versus rare gas atoms with virtually the same ionization potentials. In comparing N2+ to Ar+, a higher ion signal is seen in N2+ compared to Ar+ for linear polarization but the difference vanishes in circularly polarized light. In comparing O2+ to Xe+, we observe a suppression in O2+ compared to Xe+ for both linear and circular polarization but this suppression exhibits an intensity dependence; i.e., there is little suppression for O2+ at the lowest intensity range, but the suppression becomes increasingly stronger as the laser intensity increases. The multielectron screening model is used to discuss possible mechanisms of this intensity dependent suppression in O2+ in the multiphoton ionization regime.     

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.     

Control of cluster multielectron ionization in ultraintense laser fields

We performed classical molecular dynamics simulations to explore the controllability of the inner ionization process in Xe_n clusters (n = 2?2171), driven by ultraintense infrared Gaussian laser fields (peak intensity I _M = 10¹⁵?10¹⁸ W cm^?2, temporal pulse length τ = 10?100 fs, and frequency ν = 0.35 fs^?1). Controllability of ion charge abundances and of their spatial distributions inside the cluster emerges from the different pulse length dependences of classical barrier suppression ionization (BSI) and of electron impact ionizations (EII), as well as from the time scale of the Coulomb explosion (CE). For large clusters (Xe₂₁₇₁), low intensities (10¹⁵ W cm^?2), and long pulses (τ = 100 fs), EII is the dominating ionization channel, which favors the formation of maximum charged ions (Xe¹⁰⁺, Xe¹¹⁺) in the cluster center. In contrast, BSI forms an inverse radial charge ordering with the highest charges in the exterior cluster shells. This suggests that the production of the two inverse radial charge distributions with an equal average ion charge can be forced by the choice of multiple pulses with different intensities and pulse lengths. At high intensities (10¹⁷?10¹⁸ W cm^?2), where EII is insignificant and CE sets in much earlier, the BSI radial charge ordering and the enhancement of the ion charges beyond the single-atom limit by the ignition effect is observed only for short pulses.     

Features of the energy spectra of photoelectrons at the atomic ionization in a two-color laser field of first and third harmonics

Classical analysis and quantum-mechanical studies of the energy spectra of photoelectrons have been carried out for above-threshold ionization of atoms in a two-color laser field of the first and third (n = 3) harmonics. Numerical computations show that the boundary of direct ionization plateau corresponds to the electron energy E ≈ 3.56 \(U_{p_1 } \), while the boundary of rescattering plateau corresponds to the electron energy E ≈ 16.62 \(U_{p_1 } \) for the two-color field of fundamental frequency and its third harmonic with equal intensities, which is in accordance with the results of classical analysis. The results of classical analysis of the ionization processes in the field of first and nth harmonics of equal intensities show that the length of the direct ionization plateau and the length of the high-energy rescattering plateau decrease with increasing n. The results of numerical analysis of the ionization processes in the field of first and third (n = 3) harmonics correspond to the results of classical analysis carried out by the authors.     

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。     

Complex dynamics of correlated electrons in molecular double ionization by an ultrashort intense laser pulse

With a semiclassical quasistatic model we achieve insight into the complex dynamics of two correlated electrons under the combined influence of a two-center Coulomb potential and an intense laser field. The model calculation is able to reproduce experimental data of nitrogen molecules for a wide range of laser intensities from the tunneling to the over-the-barrier regime, and predicts a significant alignment effect on the ratio of double over single ion yield. The classical trajectory analysis allows us to unveil subcycle molecular double ionization dynamics.     

Multistep ionization of argon clusters in intense femtosecond extreme ultraviolet pulses

The interaction of intense extreme ultraviolet femtosecond laser pulses (lambda = 32.8 nm) from the FLASH free electron laser (FEL) with clusters has been investigated by means of photoelectron spectroscopy and modeled by Monte Carlo simulations. For laser intensities up to 5x10(13) W/cm(2), we find that the cluster ionization process is a sequence of direct electron emission events in a developing Coulomb field. A nanoplasma is formed only at the highest investigated power densities where ionization is frustrated due to the deep cluster potential. In contrast with earlier studies in the IR and vacuum ultraviolet spectral regime, we find no evidence for electron emission from plasma heating processes.     

Multielectron effects on single-electron strong field ionization

An apparently simple phenomenon of single-electron strong field ionization involves subtle factors related to multielectron effects. A single electron in an atom or molecule can feel a distinctly different screening strength when exposed to strong fields as opposed to weak fields, and this electron screening due to multielectron motion influences single-electron ionization. The concept and a corresponding model developed in the paper allow a generalization of the Ammosov-Delone-Krainov model for predicting strong field ionization rates of more complicated atoms and molecules. This general approach explains the recently observed anomalous low single ionization rate in O2.     

The multielectron dissociative ionization dynamics of N2 molecule in intense femtosecond laser fields with arbitrary polarization

The field-ionization Coulomb explosion model is extended to investigate the multielectron dissociative ionization process of N₂ molecule irradiated by an intense femtosecond laser field with an arbitrary polarization. The ionization process of N₂ molecule is found to be optimal at the critical internuclear distance R_c=7a.u., which is independent of the laser polarization state, the molecular explosion channel and the angle between the molecular axis and the direction of laser electric field. The kinetic energies of the ion fragments are identical in the cases of linear and circular polarizations at the same incident laser intensity. However,the probability of electron ionization is very sensitive to the above three parameters. At the critical distance R_c=7a.u. the angular dependence of the threshold intensity for the over-the-barrier ionization leads to the geometric alignment of molecules in the case of linear polarization. The threshold intensity in the case of circular polarization is apparently higher than that in the case of linear polarization, which can well explain the significant decrease of ionization in the case of circular polarization. The numerical calculations are compared with the experimental measurements.     

Quantum suppression of microwave ionization of Rydberg atoms at high scaled frequency

Microwave ionization of Rydberg atoms is well described as the onset of classical chaos when the microwave frequency omega is less than the Kepler frequency 1/n(3). However, when omega>1/n(3), i.e., at high scaled frequency Omega=omegan(3)>1, classical ionization is predicted to be suppressed by quantum interference, an analogue to Anderson localization in a solid. Using 17.55 GHz microwave fields we have observed the ionization of Sr Rydberg atoms in the regime 1相似文献   

低于再碰撞阈值下强激光场原子非序列双电离(英文)

在最近的实验和理论研究中,我们探讨了氩原子和氖原子在红外强激光场中低于再碰撞阈值的非序列双电离问题。在研究中,我们发现在非序列双电离过程中,氖原子的电子关联表现为在激光偏振面内肩并肩出射,而对于氩原子的电子关联行为表现为在激光偏振面内的背对背出射,我们采用三维半经典模型(考虑电子隧道电离)很好地解释了实验结果。在阈值附近,我们发现电子在激光场中的多次散射以及电子再碰撞激发后电子隧道电离是氩原子反关联行为的主要原因,而电子在激光场作用下的单次碰撞是电子关联行为的主要原因。通过测量双电离过程中产生电子的横向电子动量分布,观察到了库伦聚焦效应,我们认为这是非经典的关联行为。最后,我们给出了氩原子和氖原子在激光场中阈值的解析模型,并给出了原子的关联和反关联激光强度区域。     

超短强激光脉冲激励甲烷团簇的内电离机理

采用三维粒子动力学模拟方法研究了甲烷团簇在超短强激光脉冲激励下的爆炸动力学行为,重点讨论了几种典型的内电离机理对团簇爆炸过程中离子的价态和动能的影响.研究表明,在激光脉冲强度比较小的情况下,团簇中的原子主要是在光场作用下通过隧道电离的方式发生电离.当激光场进一步增强时,势垒压低电离是电离的主要方式.在相同的较高激光强度下,团簇更容易通过势垒压低电离达到高的电离价态.团簇发生电离后,其内部库仑电场的点火电离效应和内部滞留自由电子的碰撞电离效应也将增强团簇的再次电离过程. 关键词： 超短强激光脉冲 甲烷团簇 内电离     

Nonsequential double ionization of diatomic molecules by elliptically polarized laser pulses

Using the classical ensemble method, we investigate nonsequential double ionization （NSDI） of diatomic molecules by elliptically polarized laser pulses. The results show that the ellipticity of the laser field has a strong suppression effect on NSDI probabilities both in parallel and perpendicular alignments. The double ionization （DI） channel is commonly dominated by NSDI, and the NSDI channel changes with ellipticity. As ellipticity increases, more and more NSDIs occur through recollision excitation with subsequent field ionization （RESI）. Moreover, like the case of linear polarization, the two electrons involved in NSDI for perpendicularly aligned molecules are more likely to emit into the opposite hemispheres as compared to the case of parallel alignment. Additionally, this alignment effect increases as ellipticity increases.     

Calculation of cross sections of simultaneous ionization in ion-atom collisions by the generalized geometrical model

The geometrical model (GM) of ionization in ion—atom collisions [8, 9] was generalized to describe ionization of both colliding particles (simultaneous ionization) due to electron—electron interaction. The generalized GM (GGM) allows calculation of the cross sections for electron loss by an incident particle with simultaneous target ionization at collision velocities higher than characteristic electron velocities, accurate within a factor of two with respect to the Born or impulse approximation. An advantage of the GGM, except for its simplicity, is easy calculation of p(b) (p is the ionization probability and b is the impact parameter), which makes it possible to include the contribution of simultaneous ionization into more general approximate schemes for calculating cross sections of multielectron ionization of atoms or ions.