Observation of direct dissociative ionization in molecular hydrogen

Direct dissociative ionization is the simplest three-body breakup process in H2. We describe the experimental verification of direct dissociative ionization to the repulsive A2Sigma(+)(u) state by resolving the kinetic energy and angular distributions of the formed protons. A (2+1) resonant enhanced multiphoton ionization process via the isotropic E,F (1)Sigma(+)(g)(v = 6,J = 0) level is employed. The structure in the kinetic energy spectrum is well described by a projection of the vibrational wave function of the E,F (1)Sigma(+)(g)(v = 6,J = 0) state onto the repulsive ionic state. The electronic character of the ionization continuum is revealed by the proton angular distribution.     

Enhancement and control of H2 dissociative ionization by femtosecond VUV laser pulses

We report ab initio calculations of H2 ionization by VUV/fs 10(12) W/cm2 laser pulses including correlation and all electronic and vibrational degrees of freedom (DOF). Inclusion of the nuclear DOF leads to a substantial increase of resonance enhanced multiphoton ionization. By varying pulse duration, it is possible to control the ratio of dissociative to nondissociative ionization as well as the final H+(2) vibrational distribution. For pulses longer than 10 fs and proportional to omega>0.46 a.u., dissociative ionization entirely dominates, which is a very unusual situation in photoionization studies.     

Coincident fragment detection in strong field photoionization and dissociation of H2

Electron-ion momentum spectroscopy is used to investigate the correlated electronic and nuclear motion in fragmentation of H2 in 4 x 10(14) W/cm(2), 25 fs laser pulses at 795 nm. Reaction channel dependent photoelectron spectra indicate that besides the main, stepwise H2 ionization H2(+) dissociation mechanism resulting in the products H(1s) + H(+) + e(-) a second new mechanism has to be assumed. The momentum distribution of H(+) ions in the dissociation channels H(1s) + H(+) + e(-) and 2H(+) + 2e(-) is found to be independent of the kinetic energy of the photoelectrons.     

Double Ionization Dynamics of Molecular Hydrogen in Ultrashort Intense Laser Fields

We experimentally investigate the double ionization of molecular hydrogen subjected to ultrashort intense laser pulses.The total kinetic energy release of the two coincident H~+ ions,which provides a diagnosis of different processes to double ionization of H_2,is measured for two different pulse durations,i.e.,25 and 5fs,and various laser intensities.It is found that,for the long pulse duration(i.e.,25 fs),the double ionization occurs mainly via two processes,i.e.,the charge resonance enhanced ionization and recollision-induced double ionization.Moreover,the contributions from these two processes can be significantly modulated by changing the laser intensity.In contrast,for a few-cycle pulse of 5fs,only the recollsion-induced double ionization survives,and in particular,this process could be solely induced by the first-return recollision at appropriate laser intensities,providing an efficient way to probe the sub-laser-cycle molecular dynamics.     

Wakefield generation by elliptically polarized femtosecond laserpulse in ionizing gases

Wakefield generation by a femtosecond laser pulse is described in the frame of the slowly varying amplitudes approximation. The amplitude of the wakefield A, is studied as a function of laser pulse and background gas parameters, and is compared with well-known results for preformed, completely ionized plasma A_p,i. It is found that the ionization processes can increase A_p as compared to A_p,i at comparatively high laser peak intensities. It is shown that the increase of the wakefield amplitude due to gas ionization is more pronounced for circularly polarized laser pulses than for linearly polarized laser pulses. The strongest enhancement of A_p in comparison with A_p,i takes place for longer laser pulses with a duration in excess of the plasma wave period when the resonant conditions for ponderomotive excitation of the wakefield are not matched. Thus, ionization processes can expand the region of parameters for efficient generation of the laser wakefields     

飞秒激光激发空气电离的阈值研究

报道在脉宽50fs—22ps，波长800nm脉冲激光作用下的空气电离阈值的研究结果.利用探测等离子体发光信号的方法，实验测量了激发空气电离所需的阈值激光强度.结果表明，当激光脉冲宽度从50fs增加到22ps时，阈值光强I_th从8.7×10¹⁴W/cm²下降到2.7×10¹³W/cm²；I_th经历了由迅速降低逐渐发展为缓慢降低的过程.在50fs—1p     

飞秒激光激发空气电离的阈值研究

报道在脉宽50fs—22ps,波长800nm脉冲激光作用下的空气电离阈值的研究结果.利用探测等离子体发光信号的方法,实验测量了激发空气电离所需的阈值激光强度.结果表明,当激光脉冲宽度从50fs增加到22ps时,阈值光强I_th从8.7×10¹⁴W/cm²下降到2.7×10¹³W/cm²;I_th经历了由迅速降低逐渐发展为缓慢降低的过程.在50fs—1p 关键词： 飞秒激光 阈值 多光子电离 碰撞电离     

高频激光脉宽对原子光电子发射谱的影响

采用广义含时伪谱方法数值求解原子在激光脉冲作用下的动量空间含时薛定谔方程,研究了高频激光脉宽对原子光电子发射谱的影响.数值模拟表明,随着激光脉冲宽度的增加,光电子谱干涉结构的振荡幅值逐渐减小,其最大峰值的强度和位置取决于产生有效电离的最大即时强度.通过分析光电子谱的变化规律能进一步加深对高频强场电离产生的动力学干涉效应的理解.     

Evolution of photoelectron angular distributions in a train of identical,circularly polarized few-cycle laser pulses

Photoelectron angular distribution (PAD) of atoms irradiated by a train of identical, circularly polarized few-cycle laser pulses is studied in the frame of a nonperturbative scattering theory. Our study shows that the PADs vary with the kinetic energy of photoelectron, the carrier-envelope phase, and the pulse duration. We find that along with increasing of the kinetic energy of photoelectron or with decreasing of the pulse duration or the both, the original one maximum of PAD splits into two maxima; the newly produced two maxima evolve to the opposite pole of the symmetric axis, and finally incorporate as a new maximum located in the symmetric axis.Received: 26 February 2004, Published online: 10 August 2004PACS: 32.80.Rm Multiphoton ionization and excitation to highly excited states (e.g., Rydberg states) - 42.50.Hz Strong-field excitation of optical transitions in quantum systems; multiphoton processes; dynamic Stark shift - 42.65.Re Ultrafast processes; optical pulse generation and pulse compression     

Rescattering double ionization of D2 and H2 by intense laser pulses

We have measured momentum spectra and branching ratios of charged ionic fragments emitted in the double ionization of D2 (and H2) molecules by short intense laser pulses. We find high-energy coincident D+ (and H+) ion pairs with kinetic energy releases between 8 and 19 eV which appear for linearly polarized light but are absent for circularly polarized light. The dependence on the polarization, the energy distributions of the ions, and the dependence on laser intensity of yield ratios lead us to interpret these ion pairs as due to a rescattering mechanism for the double ionization. A quantitative model is presented which accounts for the major features of the data.     

Electron and Chemical Kinetics in the Low-Pressure RF Discharge Etching of Silicon in SF6

Monte Carlo simulation and Boltzmann equation solutions have been used to study the electron kinetics. All electronic excitation of SF6 is assumed to be dissociative in analogy with the known product channels in ionization and multiphoton dissociation. The electric-field-to-gas-density ratios are high (E/n ? 1000 Td, where 1 Td (Townsend) = 1 × 10-17 V . cm2) in low-pressure (p < 0.3 torr) radiofrequency (RF) discharges. At these high E/n values, the electron energy relaxation time is much shorter than the 74-ns period at 13.56 MHz. Furthermore, the time scale of the chemical kinetics is much longer than the period of the applied RF voltage. Therefore the electron energy distribution can "track" the time-varying electric field, and time- and space-averaged rate coefficients can be used in chemical kinetics models. A rate equation model has been used to study the chemical kinetic processes. Electron-impact dissociation and ionization are the dominant sources of chemically active species. An electron density of 1 × 108 cm-3 is estimated from the known average values of E/n and the discharge input power. Two limiting cases are studied for the positive and negative ion diffusion losses: a) trapped negative ions and positive ion loss at the ambipolar diffusion rate; and b) positive and negative ion losses at the free diffusion rates. Neutral particle diffusion losses are estimated by using an effective diffusion length which takes surface reflection into account and increases as the surface reflection probability increases.     

Generation of sub-mJ terahertz pulses by optical rectification

Recent theoretical calculations predicted an order-of-magnitude increase in the efficiency of terahertz pulse generation by optical rectification in lithium niobate when 500 fs long pump pulses are used, rather than the commonly used ~100 fs pulses. Even by using longer than optimal pump pulses of 1.3 ps duration, 2.5× higher THz pulse energy (125 μJ) was measured with 2.5× higher pump-to-THz energy conversion efficiency (0.25%) than reported previously with shorter pulses. These results verify the advantage of longer pump pulses and support the expectation that mJ-level THz pulses will be available by cooling the crystal and using large pumped area.     

Electron energy spectrum in the field-ionized plasma

In this article, the effect of ionization on the energy spectrum of electrons within the interaction of a laser pulse with hydrogen atoms is investigated using particle-in-cell simulation codes. The results show that the behaviour of electrons' energy distribution function in the field-ionized plasma, which occurred due to the field ionization, compared with that in the pre-plasma strongly depends on the pulse shape. For short rise-time pulses (here 30 fs), due to the rapid enhancement of laser electric field, ionization occurs quickly, and as a result, there is not much difference in the electron energy in both the media. However, for pulses with rise time of 40 fs, in the pre-plasma state, the electron population reaches higher energies compared with the field-ionized plasma state. The main reason for this difference is the nonlinear wave breaking that happens earlier due to density inhomogeneity in the field-ionized plasma. On the other hand, at longer rise-time pulses (here 60 and 70 fs), electrons achieve higher energies in the field-ionized plasma than those in the case of pre-plasma. In this case, because of density fluctuations in the field-ionized plasma, the Raman backscattered radiations are seeded by a strong initial noise at the earlier times and the Mendonca condition for chaos threshold is met sooner. Therefore, the electrons gain more energy through the stochastic mechanism that is in agreement with chaotic nature of the motion.     

Excitation and ionization of sodium clusters by a strong electromagnetic field

This paper reports on a study of the excitation and ionization of small sodium clusters by femtosecond light pulses with a maximum intensity of 5×10¹²–1×10¹⁴ W/cm² and photon energy from 1 to 3 eV made in terms of the density functional theory and jellium model through direct numerical solution of the Kohn-Sham time-dependent equation. The dependence of the degree of ionization on the intensity, duration, and frequency of the light pulses, as well as on the cluster size, is studied. The efficiency of the processes is shown to be determined primarily by the field intensity rather than by the total pulse energy.     

Coulomb explosion of large polyatomic molecules assisted by nonadiabatic charge localization

The electron-nuclear dynamics of the Coulomb explosion of a large polyatomic molecule, anthracene, is probed using kinetic energy distributions of produced H+ ions. The kinetic energy release of ejected protons exceeds 30 eV for anthracene exposed to 10(14) W cm(-2), 800 nm pulses of 60 fs duration. We propose a strong-field charge localization model, based on nonadiabatic dynamics of charge distribution in a (multiply) ionized molecule; the charge localization lasts many laser periods and is sustained through successive ionizations of the molecular ion. The model explains quantitatively the dependence of the H+ kinetic energy on the laser intensity. Dissociative ionization of a polyatomic molecule enabled by long-lived charge localization is a new type of electron-nuclear dynamics and is essential for understanding the pathways of molecular or ionic fragmentation in strong fields.     

电荷共振增强电离和离解电离在H~+_2谐波辐射中的贡献

理论研究了电荷共振增强电离和离解电离在H~+_2谐波辐射中的贡献.结果表明:在少周期激光场下,谐波辐射只由电荷共振增强电离贡献产生,谐波光谱呈规则的奇次谐波.在多周期激光场下,谐波辐射由电荷共振增强电离和离解电离共同贡献产生,但是电荷共振增强电离在谐波辐射中起主要作用.并且低阶谐波呈现偶次谐波.最后,通过分析含时核运动,电离几率以及谐波辐射时频分析图解释了少周期和多周期激光场驱动H~+_2辐射谐波的过程.     

Electron dynamics triggered by double attosecond pulses: Simulations based on time-dependent density functional theory

In order to observe the high-field effect, the external laser field must reach its peak intensity before the electron ionization. To this end, it is important to reduce pulse duration to typical attosecond timescale. In this paper, the interaction electron dynamics between attosecond pulses and dielectric is investigated within the time-dependent density functional theory. Taking the CaF₂ crystal as an example, we give a comparison of electron dynamics response between single and double pulses. Moreover, the nonlinear energy absorption and electron excitation processes are simulated by adjusting the polarization direction of the sub-pulse. Present results demonstrate that the double pulses show lower electron excitation and energy absorption than the single pulse, which is in accordance with experimental higher ablation threshold and smaller heat-affected zones of the double pulses. In addition, the curves of final excited electron number and energy absorption exhibit the quasi-symmetry about the axis of 180°, which has not been reported yet.     

超短强激光脉冲与H2＋相互作用研究：经典与量子计算的比较

用经典动力学和量子力学方法分别研究了Ｈ２＋在超短强激光场中的电离、离解和残存行为，得到了相似的结果：即在超短强激光脉冲作用下，Ｈ２＋的电离占优，但有限的量子计算低估了Ｈ２＋的离解几率；而经典处理则没有显示Ｈ２＋在超强场中的稳定化。另外，经典计算表明当核间距Ｒ伸展到一定范围时，Ｈ２＋的电离率最大。这符合量子计算中发现的电荷谐振增强电离（ＣＲＥＩ）现象。     

Routes to control of H2 Coulomb explosion in few-cycle laser pulses

We have measured coincident ion pairs produced in the Coulomb explosion of H2 by 8-30 fs laser pulses at different laser intensities. We show how the Coulomb explosion of H2 can be experimentally controlled by tuning the appropriate pulse duration and laser intensity. For laser pulses less than 15 fs, we found that the rescattering-induced Coulomb explosion is dominated by first-return recollisions, while for longer pulses and at the proper laser intensity, the third return can be made to be the major one. Additionally, by choosing suitable pulse duration and laser intensity, we show H2 Coulomb explosion proceeding through three distinct processes that are simultaneously observable, each exhibiting different characteristics and revealing distinctive time information about the H2 evolution in the laser pulse.     

Subcycle electron emission in sequential double ionization by elliptical laser pulses

Using a classical ensemble method, we have investigated sequential double ionization (SDI) of Ar atoms driven by elliptical laser pulses. The results show that the ion momentum distribution of the Ar atoms depends strongly on the pulse duration. As the pulse duration increases, the ion momentum distribution changes from two bands to four bands and then to six bands and finally to an eight-band structure. Back analysis of double ionization trajectories shows that the variation of the band structure originates from pulse duration dependent multiple ionization bursts of the second electron. Our calculations indicate that the subcycle electron emission in the SDI could be more easily accessed by using elliptical laser pulses with a longer wavelength. Moreover, we show that there is good correspondence between the scaled radial momentum and the ionization time.