TDDFT study of excitation of water molecules with short laser pulses

We explore the excitation of water molecules subject to short and intense laser pulses in the frame of time-dependent density function theory (TDDFT) at the level of the time-dependent local-density approximation (TDLDA), applied to valence electrons, coupled non-adiabatically to molecular dynamics (MD) of ions. We first study the optical absorption spectra of the water molecule as an observable in the "linear" domain and results are in good agreement with experiments. We then explore the influence of the laser frequency on the excitation. It is found that when the laser frequency is off-resonant or highly above the resonant region, the excitations are weak whereas for the resonant frequency case, the ionization is enhanced and bond lengths are enlarged. Furthermore, a direct coupling of ions with the laser pulse with the off-resonant frequency is found when investigating the OH bond lengths. We finally study the effect of laser intensity on the excitation of H 2 O and it is found that ionization increases when the laser intensity varies from low to high and we observe stable vibrations to Coulomb fragmentation when the ionization is up to typically two more charge units.     

Laser-cluster-interaction in a nanoplasma-model with inclusion of lowered ionization energies

The interaction of intense laser fields with silver and argon clusters is investigated theoretically using a modified nanoplasma model. Single pulse and double pulse excitations are considered. The influence of the dense cluster environment on the inner ionization processes is studied including the lowering of the ionization energies. There are considerable changes in the dynamics of the laser-cluster interaction. Especially, for silver clusters, the lowering of the ionization energies leads to increased yields of highly charged ions.     

CO分子在线性极化飞秒激光场中的TDDFT研究

本文运用将含时密度泛函理论和分子动力学非绝热耦合的方法,研究了CO分子在不同强度、不同极化方向的激光场中的电离和动力学行为. 研究发现,激光强度越强,CO分子吸收的能量越多,电离越早且电离越强,CO分子键长变长且伸缩振动越剧烈. 此外,CO分子偶极矩的变化及峰值也随着激光强度的增强而增大. 对激光极化方向的研究发现,激光极化方向沿着CO分子轴向时,分子的电离最强且伸缩振动最剧烈. 当激光极化角增大时,CO分子的电离逐渐被抑制且电子的偶极振动对激光极化方向表现出较强的依赖性. 此外研究还表明,CO分子碳原子和氧原子周围电子的弥散方式不同且与激光极化方向有关. 关键词： 含时密度泛函理论 分子动力学 分子电离     

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.     

碳分子线C5在激光场中的含时密度泛函理论研究

运用含时密度泛函理论和分子动力学相结合的方法, 研究了C₅分子线在强激光场中的电离激发.研究发现, 当考虑激光强度对C₅分子线激发的影响时, 激光强度越强, 分子吸收的能量越多, 电离也越早, 最终电离的电子也越多, 而且沿激光极化方向的偶极矩的变化及峰值也越大. 关于激光极化方向对C₅分子线激发的影响的研究表明, 当激光极化方向沿着C₅分子线轴向时, 分子的电离大大增强, x方向的激光脉冲仅能激发起x方向的偶极振荡, 而y方向的激光脉冲仅能激发起y方向的偶极振荡, 而且x方向的激光脉冲激发的偶极振荡强. 研究还表明, 当激光极化方向沿着C₅分子线轴向时, 尽管由于电离增强而导致C₅分子线C–C键振动的同步性变差, 但在两种激光极化方向情况下, C₅分子线的振动模式与中性C₅分子线的振动模式相同. 关键词： 含时密度泛函理论 分子动力学 分子电离 碳分子线     

Self-focusing, channel formation, and high-energy ion generation in interaction of an intense short laser pulse with a He jet

Using interferometry, we investigate the dynamics of interaction of a relativistically intense 4-TW, 400-fs laser pulse with a He gas jet. We observe a stable plasma channel 1 mm long and less than 30 microm in diameter, with a radial gradient of electron density approximately 5 x 10(22) cm(-4) and with an on-axis electron density approximately ten times less than its maximum value of 8 x 10(19) cm(-3). A high radial velocity of the surrounding gas ionization of approximately 3.8 x 10(8) cm/s has been observed after the channel formation, and it is attributed to the fast ions expelled from the laser channel and propagating radially outward. We developed a kinetic model which describes the plasma channel formation and the subsequent ambient gas excitation and ionization. Comparing the model predictions with the interferometric data, we reconstructed the axial profile of laser channel and on-axis laser intensity. The estimated maximum energy of accelerated ions is about 500 keV, and the total energy of the fast ions is 5% of the laser pulse energy.     

New experimental initiatives using very highly charged ions from an “electron beam ion trap”

A short review of the experimental program in highly-charged heavy ion physics conducted at the Lawrence Livermore National Laboratory Electron Beam Ion Trap (EBIT) facility is presented. The heavy-ion research, involving ions up to fully stripped U⁹²⁺, includes precision x-ray spectroscopy and lifetime studies, electron impact ionization and excitation cross section measurements. The investigations of ion-surface interactions following the impact of high-Z highly charged ions on surfaces are aimed to study the neutralization dynamics effecting the ion and the response of the surface as well. The combination of an EBIT% with a cryogenic Penning Trap (“RETRSP”) allows to conduct experiments with ultra cold (e.g. 10 K) very highly charged ions. These studies of charge exchange processes, Coulomb crystals and measurements of hyperfine transitions using laser spectroscopy are in progress.     

超短超强激光脉冲辐照超薄碳膜电离状态研究

为了进一步理解极端条件下物质的电离特性, 特别是超短超强激光脉冲辐照超薄靶时等离子体的形成与分布, 本文以超薄碳膜为例, 细致研究了超短超强激光脉冲辐照下原子的离化过程. 分析和比较了强激光场直接作用电离和靶内静电场电离等两种场致电离形式, 在碰撞电离可以忽略的情况下, 发现更多的电离份额是来自靶内静电场的电离方式. 研究了激光脉冲强度对电离的影响, 发现激光脉冲强度越强, 电离速度越快, 产生的高价态离子所占比例也越高.当激光强度为1×10²⁰ W/cm²时, 尽管该强度高于电离生成C⁺⁶所需要的激光强度阈值, 但该激光脉冲并不能将整个靶电离成C⁺⁶离子, 对此本文进行了详细的分析. 在研究激光脉冲宽度的影响时, 发现激光脉宽越小, 电离速度越快, 但越小的激光脉冲电离获得的高价态离子越少.     

Dynamics simulation on interaction of intense laser pulses with atomic clusters

Under classical particle dynamics, the interaction process between intense femtosecond laser pulses and icosahedral noble-gas atomic clusters was studied. Our calculated results show that ionization proceeds mainly through tunnel ionization in the combined field from ions, electrons and laser, rather than the electron-impact ionization. With increasing cluster size, the average and maximum kinetic energy of the product ion increases. According to our calculation, the expansion process of the clusters after laser irradiation is dominated by Coulomb explosion and the expansion scale increases with increasing cluster size. The dependence of average kinetic energy and average charge state of the product ions on laser wavelength is also presented and discussed. The dependence of average kinetic energy on the number of atoms inside the cluster was studied and compared with the experimental data. Our results agree with the experimental results reasonably well.     

Suppression of multiple ionization of atomic ions in intense ultrafast laser pulses

The interaction of an intense laser field with a beam of atomic ions has been investigated experimentally for the first time. The ionization dynamics of Ar+ ions and Ar neutrals in a 60 fs, 790 nm laser pulse have been compared and contrasted at intensities up to 10(16) W cm-2. Our results show that nonsequential ionization from an Ar+ target is strongly suppressed compared with that from the corresponding neutral target. We have also observed for the first time the strong field ionization of high lying target metastable levels in the Ar+ beam.     

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     

超强激光场物理学

首先,评述了超强激光场的理论结果;其次,描述了超短光脉冲在密的气体和光学介质传播中的自作用;第三,评述了强场离化无碰撞等离子体中高度离化的离子产生,及高功率超短激光脉冲巨大强度的电场可用于电子加速;第四,分析了超短声脉冲和无线电脉冲的产生和应用,讨论了在不同条件下,激光辐射谐波和 Ｘ 射线激光的产生,进一步评述了超强激光脉冲与凝聚靶相互作用可以产生接近星体物质参数的高温、超密、强磁场和巨大压力等离子体;最后,简要叙述了激光激发核、核反应,高能电子─光子相互作用的可能效应及可能进行的实验。     

超强激光场物理学

首先,评述了超强激光场的理论结果;其次,描述了超短光脉冲在密的气体和光学介质传播中的自作用;第三,评述了强场离化无碰撞等离子体中高度离化的离子产生,及高功率超短激光脉冲巨大强度的电场可用于电子加速;第四,分析了超短声脉冲和无线电脉冲的产生和应用,讨论了在不同条件下,激光辐射谐波和 Ｘ 射线激光的产生,进一步评述了超强激光脉冲与凝聚靶相互作用可以产生接近星体物质参数的高温、超密、强磁场和巨大压力等离子体;最后,简要叙述了激光激发核、核反应,高能电子─光子相互作用的可能效应及可能进行的实验。     

Excitation in ion-atom collisions inside subfemtosecond laser pulses

We discuss new excitation mechanisms in energetic ion-atom collisions embedded in short laser pulses. For comparable duration and strength of the pulse and collisional interaction, the laser field will probe and modify the interaction between projectile and target. Coherence effects emerge, insight into reaction dynamics is gained, and new dynamical features are discovered. As an example, we show (i) how a propensity rule for s-p excitation can be dramatically changed, and (ii) how the presence of the laser pulse modifies the ionization process in ion-atom collisions.     

Time resolved study of superelastic collisions in laser excited strontium vapor

We present a time-resolved experimental study of ionization by superelastic collisions in excited strontium vapor. Using short duration laser pulses for resonant excitation, we clearly observe that a delay time is necessary to reach runaway collisional ionization after the end of laser excitation.     

分子对飞秒激光场响应的含时密度泛函理论研究

采用含时密度泛函理论方法研究线性分子碳化锂(Li2C2)对飞秒激光场响应的电子-离子动力学行为.在典型的近共振和非共振的激光频率作用下,分别对比分析了分子的共振和非共振电离过程.研究发现:分子在共振频率激光场的作用下发生更强的电离过程,并倾向于发生库伦爆炸,键长的振荡断裂与电离相互促进影响,而分子在较弱的激光场作用下发生单光子电离过程;随着双脉冲时间间隔的增加,离化电子数在一定范围内呈振荡上升趋势,随后趋于常数.     

分子对飞秒激光场响应的含时密度泛函理论研究

采用含时密度泛函理论方法研究线性分子碳化锂（Li2C2）对飞秒激光场响应的电子-离子动力学行为。在典型的近共振和非共振的激光频率作用下,分别对比分析了分子的共振和非共振电离过程。研究发现：分子在共振频率激光场的作用下发生更强的电离过程,并倾向于发生库伦爆炸,键长的振荡断裂与电离相互促进影响,而分子在较弱的激光场作用下发生单光子电离过程;随着双脉冲时间间隔的增加,离化电子数在一定范围内呈振荡上升趋势,随后趋于常数。     

飞行时间质谱峰值的漂移

飞行时间质谱仪(time-of-flight mass spectrometer, TOF-MS)在分子团簇的激光电离/解离动力学研究中广泛使用。文章报道了在用脉冲355 nm的YAG激光进行水/甲醇二元团簇的多光子电离研究中,发现在电离激光相对于脉冲分子束的不同延时下,即激光作用于脉冲束的不同位置,飞行时间质谱仪测得的离子的质谱峰值发生漂移。在激光作用于脉冲束的中段时,离子的信号最强,同时离子的峰值漂移达到最大。分析认为：这种峰值漂移不是因为新质量数谱峰的出现,而是离子在穿越质谱仪的离子引出区和加速区极板时发生部分离子吸附,引起极板间电压的起伏造成的。离子在电场起伏下的数值模拟与实验中观测到的离子峰值漂移规律一致。