异核双原子和三原子分子在红外强激光场中的电离抑制

Ionization is the fundamental process in interaction of atoms/molecules with femtosecond strong laser fields. Comparing to atoms, molecules exhibit peculiar behaviors in strong-field ionization because of their diverse geometric structures, molecular electronic orbitals as well as extra nuclear degrees of freedom. In this study, we investigate strong field single and double ionization of carbon monoxide (CO) and carbon dioxide (CO₂) in linearly polarized 50-fs, 800-nm laser fields with peak intensity in the range of 2×10¹³ W/cm² to 2×10¹⁴ W/cm² using time-of-flight mass spectrometer. By comparing the ionization yields with that of the companion atom krypton (Kr), which has similar ionization potential to the molecules, we investigate the effect of molecular electronic orbitals on the strong-field ionization. The results show that comparing to Kr, no significant suppression is observed in single ionization of both molecules and in non-sequential double ionization (NSDI) of CO, while the NSDI probability of CO₂ is strongly suppressed. Based on our results and previous studies on homonuclear diatomic molecules (N₂ and O₂), the mechanism of different suppression effect is discussed. It is indicated that the different structure of the highest occupied molecular orbitals of CO and CO₂ leads to distinct behaviors in two-center interference by the electronic wave-packet and angular distributions of the ionized electrons, resulting in different suppression effect in strong-field ionization.     

Effect of tunneling ionization on dynamic alignment and post-ionization alignment of nitrogen molecules irradiated by different laser intensities

The dynamic alignment and post-ionization alignment of nitrogen molecules are investigated while considering the effect of tunneling ionization. The effects of tunneling ionization on the angular distribution are calculated when the molecules are irradiated by different laser intensities. The results show that laser intensity directly affects the time and extent of dynamic alignment. Furthermore, the extent of post-ionization alignment is not only determined by laser intensity but also affected by the final extent of dynamic alignment. The post-ionization alignment will dominate during the process of molecular (or molecular ion) rotational alignment for femtosecond laser pulse. The time of tunneling ionization is a significant factor to the final ensemble angular distribution of molecular ions when laser intensity is low.     

Collective multielectron tunneling ionization in strong fields

We investigate the quantum mechanical process of two-electron tunneling in strong external electric fields. Numerical solution of a two-electron s-wave model reveals the existence of collective tunneling ionization in a mode where both electrons stay at equal distance from the nucleus. Otherwise the lagging electron is immediately recaptured. The corresponding double ionization rate fails to explain nonsequential multiple ionization in strong-field laser experiments. However, an empirically modified version of the analytical one-electron tunneling rate of Ammosov, Delone, and Krainov agrees with the experiments to a surprising accuracy. The reason for this agreement is presently unknown.     

Excitation of He atoms in the strong-field tunneling regime

We report on strong-field excitation of He atoms with two interfering laser pulses of various polarization. The results are explained within the frustrated tunneling ionization model which describes multi-photon excitation in the strong-field tunneling regime.     

Effects of molecular structure on ion disintegration patterns in ionization of O2 and N2 by short laser pulses

We demonstrate that the structure of the outermost orbitals of oxygen and nitrogen can be observed in the angular distribution of coincident ion pairs generated by the double ionization of these molecules by 8 fs laser pulses. We do this by establishing that these ions emerge from well defined excited electronic states of O2+2 and N2+2 respectively and that they are produced dominantly through a process which involves electron rescattering. The angular distributions of the ions from the two targets are very different, reflecting the different structures of the outermost orbitals of the two molecules.     

Quantum interference of multi-orbital effects in high-harmonic spectra from aligned carbon dioxide and nitrous oxide

We investigate experimentally multi-orbital effects in high-order harmonic generation(HHG) from aligned CO_2 and N_2O molecules by intense femtosecond laser fields with linear and elliptical polarizations.For either of the aligned molecules, a minimum in the harmonic spectrum is observed, the position of which shifts to lower-order harmonics when decreasing the intensity or increasing the ellipticity of the driving laser.This indicates that the minimum originates from the dynamic interference of different channels, of which the tunneling ionization and recombination are contributed via different molecular orbitals.The results show that both the highest occupied molecular orbital(HOMO) and low-lying HOMO-2 in CO_2(or HOMO-1 in N_2O) contribute to the molecular HHG in both linearly and elliptically polarized strong laser fields.Our study would pave a way for understanding multi-electron dynamics from polyatomic molecules irradiated by strong laser fields.     

Tunneling ionization of a hydrogen atom in short and ultrashort laser pulses

The ionization of a hydrogen atom in a linearly polarized low-frequency electromagnetic field is investigated by direct numerical integration of the time-dependent Schrödinger equation. The data obtained for various ionization regimes and various initial atomic states are compared with the Keldysh and Perelomov-Popov-Terent’ev (PPT) theories. The validity ranges for the quasi-static model of tunneling ionization and the PPT theory in laser intensity and frequency are determined. The tunneling ionization of the excited 2s and 2p states is discussed. The ionization of a hydrogen atom in an ultrashort (on the order of one optical period) pulse is investigated.     

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.     

Angular momentum distribution in strong-field frustrated tunneling ionization

Using the classical-trajectory Monte Carlo model, we have theoretically studied the angular momentum distribution of frustrated tunneling ionization(FTI) of atoms in strong laser fields. Our results show that the angular momentum distribution of the FTI events exhibits a double-hump structure. With this classical model, we back traced the tunneling coordinates, i.e., the tunneling time and initial transverse momentum at tunneling ionization. It is shown that for the events tunneling ionized at the rising edge of the electric field,the final angular momentum exhibits a strong dependence on the initial transverse momentum at tunneling.While for the events ionized at the falling edge, there is a relatively harder recollision between the returning electron and the parent ion, leading to the angular momentum losing the correlation with the initial transverse momentum. Our study suggests that the angular momentum of the FTI events could be manipulated by controlling the initial coordinates of the tunneling ionization.     

Theoretical study of processes of multiple excitation/ionization in K-photoabsorption of carbon and nitrogen in CO and N2 molecules

Spectra of multiple excitation/ionization in the region of photoabsorption K-edge of carbon and nitrogen of CO and N₂ molecules in the gas phase are studied theoretically. Processes of additional excitation/ionization from the 1π-and 5σ shells are taken into account. Single-electron wave functions in the excited state are calculated allowing for the effect of core wave functions in the field of a vacancy by the single-center method in the Hartree-Fock approximation. Cross sections for photoabsorption are calculated using the theory of nonorthogonal orbitals. The influence of many-electron correlations on the extension of the multiplet structure of certain configurations of multiple excitation is studied.     

7.87 eV postionization of peptides containing tryptophan or derivatized with fluorescein

Chemical tags such as anthracene can be attached to a molecular analyte and serve as chromophores for 7.87 eV laser postionization by lowering the overall ionization potential of the tagged molecular complex. Fluorescein and tryptophan are demonstrated as two new tags for 7.87 eV laser postionization of various amino acids and peptides. Other molecular species that are efficient fluorescence probes should also serve as tags for 7.87 eV postionization since they display highest occupied molecular orbitals with extended π-conjugation that lead to ionization potentials below this photon energy and an ability to stabilize the net positive charge of the radical cations. This technique is demonstrated here for laser desorbed species, but is also applicable to keV ion sputtered neutrals. Overall, 7.87 eV laser postionization of derivatized species promises to expand the capabilities of mass spectrometric surface analysis.     

Interference oscillations in the angular distribution of laser-ionized electrons near ionization threshold

We analyze the two-dimensional momentum distribution of electrons ionized by few-cycle laser pulses in the transition regime from multiphoton absorption to tunneling by solving the time-dependent Schr?dinger equation and by a classical-trajectory Monte-Carlo simulation with tunneling (CTMC-T). We find a complex two-dimensional interference pattern that resembles above threshold ionization (ATI) rings at higher energies and displays Ramsauer-Townsend-type diffraction oscillations in the angular distribution near threshold. CTMC-T calculations provide a semiclassical explanation for the dominance of selected partial waves. While the present calculation pertains to hydrogen, we find surprising qualitative agreement with recent experimental data for rare gases [A. Rudenko, J. Phys. B 37, L407 (2004)].     

Multiphoton and tunneling ionization of atoms in an intense laser field

We study the ionization probabilities of atoms by a short laser pulse with three different theoretical methods,i.e.,the numerical solution of the time-dependent Schro¨dinger equation(TDSE),the Perelomov-Popov-Terent’ev(PPT) theory,and the Ammosov-Delone-Krainov(ADK) theory.Our results show that laser intensity dependent ionization probabilities of several atoms(i.e.,H,He,and Ne) obtained from the PPT theory accord quite well with the TDSE results both in the multiphoton and tunneling ionization regimes,while the ADK results fit well to the TDSE data only in the tunneling ionization regime.Our calculations also show that laser intensity dependent ionization probabilities of a H atom at three different laser wavelengths of 600 nm,800 nm,and 1200 nm obtained from the PPT theory are also in good agreement with those from the TDSE,while the ADK theory fails to give the wavelength dependence of ionization probability.Only when the laser wavelength is long enough,will the results of ADK be close to those of TDSE.     

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     

Theory of light rectification in scanning tunneling microscopy in the presence of an adsorbed molecule

We consider the problem of the rectified current induced by laser radiation in the STM junction when the tip is placed above a small molecule like CO or NO. This is calculated assuming a simple tight-binding model for the tunneling junction including the adsorbate and using nonequilibrium Green's functions techniques. The coupling between tunneling electrons and the molecule vibrational modes is taken into account by a local electron-phonon interaction term. In a second step we estimate the excitation rate of the molecule vibrations for a given laser power. This value is then used to obtain the relative change in the rectified current when the laser is in resonance with a molecule vibration. For a moderate laser power of 2 kW/cm² a relative change of 1 to 3% is predicted.     

基于OFI椭圆偏振光场等离子体中电离电子能量分布的研究

在准静态隧道电离理论模型和准经典阈上电离理论模型的基础上,建立了一个描述基于光场感生电离的椭圆偏振光场电离电子能量分布的简单模型,推导出了既易于理解又相对简单适用的描述椭圆偏振光场的电子能量分布函数解析表达式.利用此式数值计算了不同偏振参量下的椭圆偏振光场中类钯氙系统的电子能量分布曲线,计算结果表明在相同的激光功率密度下,偏振参量对基于OFI电子碰撞机制的X射线辐射强度是有影响的,并与报道的实验结果一致 关键词： 椭圆偏振光场 电子能量分布 类钯氙系统 电子碰撞机制     

Selective steering of molecular multiple dissociative channels with strong few-cycle laser pulses

We report that multiple dissociative channels of carbon monoxide (CO) molecules are selectively controlled using intense phase-stabilized few-cycle laser fields (4.2 fs, 740 nm, 6×10(14) W/cm(2)). The controllable emission direction of C(2+) from charge asymmetrical dissociation and ionization of CO dications is out of phase in a linear polarized laser field. The strong coupling between the channels is explained as the competition of recollision excitation and recollision ionization in a recollision process, leading to the opposite asymmetrical property. The experimental result provides insight into high degree controlling molecular multiple dissociative processes in the time scale of electronic motion.     

Observation of a transition in the dynamics of strong-field double ionization

The double ionization of argon and xenon in an intense laser field has been studied in detail using an electron-ion coincidence technique. The observed double ionization electron spectra in xenon show resonancelike structures here resolved for the first time. In argon, the featureless spectra are consistent with rescattering. This represents a clear transition in the dynamics of strong-field double ionization, analogous to the well-known transition between the tunneling and multiphoton regimes in single ionization.     

强激光场原子隧道电离的研究新进展

光与物质的相互作用一直是科学的主旋律之一.随着超强超短激光技术的快速发展,如今人们可以研究单个原子的内部世界,并调控光与电子的相互作用,从而实现了对原子内电子的超快动力学过程的探索.强激光诱导的原子隧道电离是众多强场物理现象的基石,具有重要的研究意义,也是研究前沿的热点之一.综述了强场原子隧道电离的最新研究进展,基于隧...     

Correlation between double and nonresonant single ionization

We performed simultaneous measurements of electrons and ions produced in Xe photoionization driven by an 800-nm, 100-fs laser pulse. The obtained energy and angular resolved electron spectra allow the identification of the electronic states populated during the ionization. Xe2+ ions appear at the same laser intensity as electrons emerging from a nonresonant 9-photon ionization process of Xe. Similar to optical tunneling ionization, the nonresonant ionization delivers low-energy electrons needed for the formation of Xe2+ by a backscattering process.