NO分子和氧原子的高分辨离子谱实验研究

共振增强多光子电离及飞行时间质谱技术是一种具有高分辨率、高灵敏度的光谱研究技术。利用上述技术研究了由激光光解NO2产物-NO与原子O的离子谱,获得了振转态高度分辨的NO(X^2П,v″,J″)γ(0,0)γ(0,1)γ(1,1)带的离子谱以及自旋-轨道精细能级分辨的氧原子O(2P^3PJ^″=2,1,0)离子谱。氧原子O(2P^3PJ^″=2→3P^3PJ^″、2P^3PJ^″=1→3P^3PJ′、2P^3PJ″=0→3P^3PJ′)的离子信号位于紫外电离探测激光的波长分别为225．65nm,226．04nm,226．23nm。实验表明,共振增强多光子电离加飞行时间技术研究原子、分子光谱其灵敏度与分辨率远高于常用的激光感生荧光方法。所得到的NO分子与氧原子的离子谱及它们的离子信号对NO2分子光解及NO分子与氧原子的电离动力学研究提供了有益的实验信息。     

NO(3+1)共振增强的多光子离化谱

用皮秒脉冲高功率Nd∶YAG激光器抽运的光学参量发生/放大器作激发源,获得了NO分子在420～500 nm波长范围内的多光子离化谱,光谱图呈现分离谱的特征,表明在该波长区间NO分子以多光子共振方式离化。离化信号随激光强度的近四次方变化关系表明,在420～500 nm波长范围内NO分子吸收4个光子而离化。通过对谱线的标识,首次分离出NO分子以E 2Σ激发电子态为中间共振态的(3+1)多光子离化光谱序列,由谱线序列峰值波长得到NO分子E 2Σ电子态的振动常数,从而实现了采用多光子离化技术对该态能级结构的实验研究。     

NO通过C~2Π←X~2Π跃迁的共振多光子离化谱

以皮秒Nd∶YAG激光器抽运光学参变发生 /放大器做激发源 ,得到了NO分子在 4 90～ 5 80nm波长范围内通过C2 Π态共振增强的多光子离化谱 ,离化谱由有规则的谱线序列组成。将理论计算的峰值位置与实验结果进行比较 ,确定了离化通道为 :NO(X2 Π) 3hνNO(C2 Π) 2hν(orhν) NO+ +e ,离化信号强度随激光强度的近五次方变化关系进一步验证了此结论。分析讨论了谱线强度的分布不符合夫兰克康登原理的可能原因。根据谱线峰值位置 ,利用最小二乘法拟合获得NO分子C2 Π态振动常数′ωe=(2 35 4 .9± 6 .4 )cm-1,′ωe ′χe=(14 .7± 2 .5 )cm-1及平衡位置的力常数k=(2 .4 4± 0 .0 8)× 10 3 N·m-1。结果可为用激光离化光谱技术探测大气污染物NO分子提供参考。     

410～355 nm内四甲基硅的多光子解离和电离研究

利用平行板电极装置研究了四甲基硅在410～378 nm内的MPI光谱;利用TOF质谱仪研究了该分子在402～371 nm内若干个波长点处的TOF质谱;利用四极质谱装置研究了它在355 nm处的MPI质谱.测得了355 nm下Si(CH3)+n(n=1,2,3,4)及Si+的激光光强指数,以及其信号强度占总信号强度的分支比随光强的变化关系.据此,讨论了该分子MPI过程的可能通道,得出了Si+主要来自于母体分子的多光子解离-硅原子的电离、Si(CH3)+n(n=1,2,3)主要来自于Si(CH3)n(n=1,2,3)的自电离、Si(CH3)+4来自于母体分子的(3+1)电离的结论.     

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.     

紫激光作用下四甲基硅的光谱和质谱研究

本文利用平行板电极装置及飞行时间质谱仪相结合的方法对四甲基硅进行了多光子电离（ＭＰＩ）光谱及飞行时间（ＴＯＦ）质谱的研究。得到了激光激发波长在４０２～３９２ｎｍ内的多光子电离光谱，获得了某些波长处的飞行时间质谱，并据此讨论了该分子在这个区域内可能的ＭＰＩ机理。     

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.     

Two-colour coherent control of multiphoton ionization： a comparison between long-range and short-range potential model atoms

Using the numerical solution of the time-dependent Schr\"odinger equation of a one-dimensional model atom in a two-colour laser field, we have investigated the effects of the potential models on coherent control of atomic multiphoton ionization. It is found that the photoelectron spectra are obviously different for the long-range (Coulomb-like) and short-range (with no excited bound states) potential model atoms, which are produced by two-colour coherent control of atomic multiphoton ionization in a few laser cycles. Our results indicate that two-colour coherent control of atomic multiphoton ionization can be observed in simulations, depending on the choice of the model potentials.     

丁酮分子的多光子电离-离解机理

研究了丁酮分子经(n0,3d)共振的多光子电离-离解机理(MPID).多光子电离-飞行时间质谱测得的主要离子产物是C2H3O+和CH3CH+2,C2H3O+的强度为CH3CH+2的2～5倍,还有少量C2H+2,C2H+3和CH+3离子,未见到母体离子.主要离子产物的分质量多光了电离谱结构相似,而各离子产物的光强指数不同.实验结果说明丁酮分子的多光子电离-离解机理符合母体离子阶梯模型,文中用梯开关模型对主要产物离子的产生机理进行了解释.     

NH_3多光子电离和裂解动力学过程分析

本文分析了在XeCl准分子激光作用下NH_3分子的多光子电离质谱形成机理。所建立的动力学模型包括主要由经过中间态(6)和(1)的(2+1)共振多光子电离,生成NH_3~+;离子-分子反应形成大量的NH_4~+;经(6)态的(2+2)共振多光子电离,可能产生低产额的NH_2~+。这个模型的速率方程解与实验测量符合得很好,并在离子流强度对激光脉冲宽度的依赖关系中预示直接电离或间接电离机制的信息。     

丙酮分子的分质量共振多光子电离光谱及多光子电离—离解机理研究

用多光子电离飞行时间质谱法三光子与丙酮分子３ｄ形态和４ｓ态共振的激光波长区域获得了丙酮分子的共振多光子电离分质量多光子电离（ＭＰＩ）光谱和飞行时间质谱，实验观察到的主要产物是ＣＨ３ＣＯ＾＋和ＣＨ＾＋３，还观察到了少量的Ｃ＾＋，ＣＨ＾＋，ＣＨ＾＋２和ＣＨＯ＾＋，在实验的激光波长范围内未见到母体离子，分质量多光子电离光谱具有相似的光谱结构，几个主要谐峰分别对应着（ｎ０，３ｄ）和（ｎ０，４ｓ）里德堡跃迁     

Angular distributions for double ionization of Li- by an ultrashort, intense laser pulse.

We predict photoelectron angular distributions for double ionization of Li- by both weak and intense ultrashort, linearly polarized laser pulses by direct numerical integration of the three-dimensional, time-dependent Schr?dinger equation. Li- is treated as a two-active electron system. Near threshold, for low intensity we recover general features of angular distributions for one-photon double ionization. For the intense field (multiphoton) case, the photoelectron angular distribution changes significantly, particularly in directions parallel and perpendicular to the laser polarization axis.     

Probing angular correlations in sequential double ionization

We study electron correlation in sequential double ionization of noble gas atoms and HCl in intense, femtosecond laser pulses. We measure the photoelectron angular distributions of Ne+ relative to the first electron in a pump-probe experiment with 8 fs, 800 nm, circularly polarized laser pulses at a peak intensity of a few 10(15) W/cm2. Using a linear-linear pump-probe setup, we further study He, Ar, and HCl. We find a clear angular correlation between the two ionization steps in the sequential double ionization intensity regime.     

Development of laser photoelectron spectroscopy based on resonantly enhanced multiphoton ionization

This review article is mainly concerned with laser photoelectron spectroscopy based on REMPI (resonantly enhanced multiphoton ionization), consisting of two parts. One is associated with the measurement of photoelectron kinetic-energy distribution and the other is associated with the measurement of zero-kinetic-energy (ZEKE) photoelectrons in very high resolution. These two techniques are complementary to each other. During the last three decades, the author and co-workers have carried out photoelectron spectroscopic studies of molecules in the gas phase, using the HeI 584 Å resonance line and a nanosecond tunable UV–visible laser. In this article, firstly the author’s background in the field of molecular photoelectron spectroscopy is described briefly, by mentioning three topics of HeI photoelectron spectroscopy. Secondly, the principle and characteristics of laser photoelectron kinetic-energy spectroscopy and its application to several typical topics, namely, one-photon forbidden states (O₂), autoionization from a super-excited state (NO), and small van der Waals molecules (NO–Ar and the NO₂ dimer), and some others. Thirdly, the principle and characteristics of ZEKE photoelectron spectroscopy are described, together with its application to the following several topics: (1) rotational spectra of NO⁺, (2) vibrational coupling of (naphthalene)⁺, (3) large-amplitude torsional motion of (tolane)⁺, (4) rotational isomers of (cis and trans n-propylbenzene)⁺ and structural isomers of (2-hydroxypyridine)⁺, (5) proton tunneling of (tropolone)⁺ and (9-hydroxyphenalenone)⁺, (6) intramolecular vibrational redistribution of trans stilbene, and (7) cation van der Waals molecules of aniline–Ar_n (n=1,2) and azulene–Ar. All the results mentioned as examples are those obtained in the author’s laboratory.     

Strong-field double ionization of Ar below the recollision threshold

Nonsequential double ionization of Ar by 45 fs laser pulses (800 nm) at (4-7)x10;{13} W/cm;{2} was explored in fully differential measurements. Well below the field-modified recollision threshold we enter the multiphoton regime. Strongly correlated back-to-back emission of the electrons along the polarization direction is observed to dominate in striking contrast to all previous data. No effect of Coulomb repulsion can be found, the predicted cutoff in the sum-energy spectra of two emitted electrons is confirmed, and the potential importance of multiple recollisions is discussed.     

NO2分子的光学-光学双色双共振多光子离化谱

以Nd:YAG激光器的二倍频输出光为抽运光,其三倍频输出抽运的光学参量发生/放大器输出光为探测光,利用光学-光学双色双共振多光子离化光谱技术(OODR-MPI),获得了NO₂分子在605—675nm探测光波长范围内的多光子离化激发谱. 通过对NO₂分子离化机理的分析,确定了在此波长区间,NO₂分子经1+3+1双共振多光子过程离化,离化通道为NO₂(X²A₁)hν 关键词： 2')" href="#">NO₂ 光学-光学双共振多光子离化谱 里德伯态 分子常数     

Enhanced nonlinear double excitation of He in intense extreme ultraviolet laser fields

Nonlinear, three-photon double excitation of He in intense extreme ultraviolet free-electron laser fields (～24.1 eV, ～5 TW/cm2) is presented. Resonances to the doubly excited states converging to the He+ N=3 level are revealed by the shot-by-shot photoelectron spectroscopy and identified by theoretical calculations based on the time-dependent Schr?dinger equation for the two-electron atom under a laser field. It is shown that the three-photon double excitation is enhanced by intermediate Rydberg states below the first ionization threshold, giving a greater contribution to the photoionization yields than the two-photon process by more than 1 order of magnitude.     

Generation of attosecond pulses in molecular nitrogen

We investigate the carrier-envelope phase dependence of the total ionization yield for single and double ionization of xenon. We compare our results to theoretical calculations and to the phase dependent asymmetry in photoelectron emission. We observe that the phase dependence of the photoion yields, regardless if single or double ionization, is at least 2-3 orders of magnitude below the photoelectron emission signal. We conclude that total photoionization yields are only very weakly dependent on the carrier envelope phase, and that they are not a useful means for measurement of the phase. It seems possible that the broad bandwidth of few-cycle pulses facilitates multiphoton ionization, which leads to a randomization of strong field ionization phase dependencies. Besides, we observe that the spatial asymmetry in photoelectron emission appears to be useful as an indicator for the laser pulse duration in the few cycle regime.     

Multiphoton double ionization of barium

The multiphoton double ionization of Ba from ~280 to 700 nm was investigated using laser pulses 5 ns long of peak intensity ~10¹⁰ W/cm². The spectrum consists of a number of strong resonances, which can be assigned to Ba⁺ transitions. Most of the assignments have been verified by pump-probe techniques. Thus, the Ba⁺⁺ observed is due to sequential ionization. The multiphoton ionization probability is highest for λ~500 nm, which matches a series of strong Ba and Ba⁺ transitions leading to double ionization     

Dynamic Interference Photoelectron Spectra in Double Ionization:Numerical Simulation of 1D Helium

We report our numerical simulation on the dynamic interference photoelectron spectra for a one-dimensional(1D) He model exposed to intense ultrashort extreme ultraviolet(XUV) laser pulses.The results demonstrate an unambiguous interference feature in the photoelectron spectra,and the interference is unveiled to originate from the dynamic Stark effect.The interference photoelectron spectra are prompted for intense sub-femtosecond XUV laser pulses in double ionization.The stationary phase picture is corroborated qualitatively in the two-electron system.The ability of probing the dynamic Stark effect by the photoelectron spectra in a pragmatic experiment of single-photon double ionization of He may shed light on further investigation on multi-electron atoms and molecules.