Directional emission of multiply charged ions during dissociative ionization in asymmetric two-color laser fields

Intense, asymmetric 1ω+2ω laser fields are used to affect the directional ejection of multiply charged ion fragments from a variety of molecules, including N2, O2, CO, HBr, and CO2. By tuning the relative phase, ?, between the two fields, we observe large forward-backward dissociation asymmetries. The largest asymmetries are obtained at the same values of ? for all species, suggesting a common dynamical mechanism. Following an independent phase calibration, the sign of the asymmetry appears to be opposite that expected from the standard enhanced ionization model.     

Asymmetric structure of atomic above-threshold ionization spectrum in two-color elliptically polarized laser fields

According to the frequency-domain theory, we investigate the asymmetric structure of above-threshold ionization(ATI) spectrum of an atom in two-color elliptically polarized(EP) laser fields. When both laser fields are linearly polarized(LP), the spectrum shows that the multi-plateau structure is symmetric about the emitted angle of electron at π/2, while the spectrum becomes asymmetric and shifts rightwards with the increase of the EP degree of the IR laser field. Since the total ATI process is regarded as including direct ATI and the rescattering ATI, we analyze the spectrum structure of direct ATI and rescattering ATI separately. Using the saddle-point approximation, we find that for direct ATI, the fringes on the spectrum are mainly attributed to the fact that the ionization probability becomes very small when the direction of emitted electrons is perpendicular to the direction of the XUV laser polarization; while for the rescattering ATI, the interference fringes on the spectrum mainly come from the superposition of the waist structures on the spectra of all sub-channels.     

Helicity-dependent time delays in multiphoton ionization by two-color circularly polarized laser fields

By numerically solving the three-dimensional time-dependent Schrödinger equation, we have invest-tigated multiphoton ionization of hydrogen atom in the two-color circularly polarized (TCCP) laser fields consisting of a strong 400 nm and a much weaker 800 nm pulses. Due to the presence of perturb-bative 800 nm laser pulse, sideband peaks emerge between the above-threshold ionization rings in the photoelectron momentum distributions. Our numerical results show that the sideband peaks exhibit one-lobe structure in the co-rotating TCCP laser fields, while it displays the three-lobe structure in the counter-rotating TCCP laser fields. Moreover, the photoelectron yield of sidebands in the co-rotating TCCP fields is much higher than those of the counter-rotating TCCP fields. These phenomena could be well explained from the perspective of the photon-absorption channels via the selection rules. In-terestingly, an obvious phase shift between the sidebands of different orders from the co-rotating and counter-rotating TCCP fields is observed. This shift indicates the helicity-dependent time delay in the one-photon continuum-continuum transition process.     

Internal collision double ionization of molecules driven by co-rotating two-color circularly polarized laser pulses

The double ionization process of molecules driven by co-rotating two-color circularly polarized fields is investigated with a three-dimensional classical ensemble model. Numerical results indicate that a considerable part of the sequential double ionization(DI) events of molecules occur through internal collision double ionization(ICD), and the ICD recollision mechanism is significantly different from that in non-sequential double ionization(NSDI). By analyzing the results of internuclear distan...     

Dissociative ionization of molecules in intense laser fields

Accurate and efficient grid based techniques for the solution of the time-dependent Schrödinger equation for few-electron diatomic molecules irradiated by intense, ultrashort laser pulses are described. These are based on hybrid finite-difference, Lagrange mesh techniques. The methods are applied in three scenarios, namely H₂ ⁺ with fixed internuclear separation, H₂ ⁺ with vibrating nuclei and H₂ with fixed internuclear separation and illustrative results presented.Received: 19 November 2002, Published online: 24 April 2003PACS: 02.60.Cb Numerical simulation; solution of equations - 02.70.Bf Finite-difference methods - 33.80.Rv Multiphoton ionization and excitation to highly excited states (e.g., Rydberg states) - 33.80.-b Photon interactions with molecules     

Dependence of above-threshold ionization spectrum on polarization directions of two-color laser fields

Using the frequency-domain theory, we investigate the above-threshold ionization(ATI) process of an atom in twocolor laser fields. When both photon energies of the two-color laser fields are much smaller than the atomic ionization threshold, the ATI spectrum depends on the angle between the two lasers' polarization directions. While when the photon energy of one laser is comparable with or larger than the atomic ionization threshold, the ATI spectrum is independent of the angle, and only several dips appear at certain angles. By analyzing the contributions of different quantum channels, we find that, for the case that both frequencies of the two color lasers are low, the quantum interferences between the channels are strong, and hence the spectrum changes with the angle between the two lasers' polarization directions. While for the case that the frequency of one of the two color lasers is high, the contributions of the channels to the ATI spectrum decrease dramatically with increasing channel order, hence the interferences between the channels disappear, and the ATI spectrum has a step-like structure, which is independent of the angle between the two lasers' polarizations. These results can shed light on the study of the corresponding relation between classical and quantum mechanisms of the matter–laser interaction in high-frequency laser fields.     

Influence of relative phase on the nonsequential double ionization process of CO_2 molecules by counter-rotating two-color circularly polarized laser fields

We investigate the nonsequential double ionization(NSDI) of linear triatomic molecules by the counter-rotating two-color circularly polarized(CRTC) laser fields with a classical ensemble method. The results of the simulation reveal that NSDI yield strongly connected with the relative phase. The trajectory tracking method shows that the return time of the electron is controlled by the relative phase. In addition, when we change the CRTC laser wavelengths, the relative phase of the maximum and minimum yield of NSDI also changes. This shows that the influence of the Coulomb potential in the triatomic molecules on the electron return process cannot be ignored. This work will effectively promote the electronic dynamics study of NSDI for the triatomic molecule.     

Multiphoton ionization of atoms by a two-color laser pulse

The probability of multiphoton ionization of atoms in a laser radiation field containing an additional second harmonic is calculated by the imaginary time method [9, 10]. The conditions are found when the second-harmonic contribution to the ionization of atoms dominates over that of the first harmonic. It is shown that the average momentum of photoelectrons ejected from atoms depends on the phase shift between the first and second harmonics and their mutual polarization. The obtained asymptotic expressions can be used for the qualitative explanation of experiments on generation of terahertz radiation from the optical breakdown region in gas in the focus of a femtosecond laser.     

Nonlinear ionization of organic molecules in high intensity laser fields

We use a series of 23 organic molecules to study ionization of complex media caused by their interaction with intense 40 fs, 0.8 &mgr;m pulses. All molecules reach saturated ionization at higher intensities than would be expected for atoms of the same ionization potential, reminiscent to what has been reported for dielectric breakdown with femtosecond pulses. Dependence of the ionization rate on the alignment of the molecule with the laser field is ruled out as the cause of the high saturation intensities. All molecules allow a significant range of intensities between the region of approximately 100% ionization and before the second and subsequent electrons are removed.     

Effect of elliptical polarizations on nonsequential double ionization in two-color elliptically polarized laser fields

Using the classical ensemble model, we investigate the nonsequential double ionization(NSDI) of Ar and Mg in the two-color elliptically polarized laser pulse for different elliptical polarizations. Numerical results show that for Ar atoms the NSDI yield increases as the ellipticity increases, which is different from the case of Mg atoms. Moreover, the correlated behavior in the correlated electron momentum along the x direction and ion momentum distributions of Ar atoms are influenced by the ellipticity. By statistical analysis of different times, we can conclude that the ellipticity may be responsible for the NSDI processes. The correlated momenta distributions along the x direction at the recollision time are demonstrated and the results show that the travelling time and ellipticity can affect the emitted directions of both electrons.     

Controlling electron collision by counterrotating circular two-color laser fields

Electron collision as well as its controlling lies in the core of study on nonsequential double ionization(NSDI).A single collision occurred in a convergent time is important to disclose the essential features of the electron correlation.However,it is difficult to form such a collision.By using counterrotating circular two-color(CRTC)laser fields,we show that a single electron collision can be achieved in a convergent time and a net electron correlation is set up within the sub-femtosecond time scale in the NSDI process of Ar atoms.The proposed method is also valid for other atoms,provided that one chooses the frequency and intensity of the CRTC field according to a scaling law.     

Dynamics of strong-field double ionization of H_2 in co-rotating two-color circularly polarized laser fields

Double ionization of H_2 in a co-rotating two-color circularly polarized(TCCP) laser field is theoretically investigated. By changing the ratio of electric field peak amplitudes of the TCCP laser pulses, the double ionization probability as a function of the laser intensity shows a clear knee structure, which is suppressed significantly in the case of the atom. Due to the large spatial range of the electronic initial distribution, with the analysis of classical trajectories of ionized electrons, it is found that the ionization of the electron in the farther distance increases the probability of recollision. Furthermore, the yield of nonsequential double ionization created by the recollision can be enhanced by controlling the amplitude ratio of the TCCP laser field.     

双色激光场中激光强度和脉宽对线性多原子分子离子电离的影响

利用强激光场电离和离解分子来研究分子激发态的波包结构是强场物理的重要研究方向。利用短时指数传播子对称分割法和快速傅里叶变换技术,数值求解了一维含时Schr-dinger方程,探讨了双色激光场中激光的基波和谐波强度之间的不同配比以及脉宽对线性多原子分子离子电离的影响。理论计算结果表明：基波和谐波的相对相位为π时,尽管随着激光的基波和谐波强度之间配比的变化,电离几率随原子间距变化的趋势基本保持不变,但在一定的激光基波强度下（1.2×1013~1.2×1015 W/cm2),激光基波强度的变化可以明显改变电离几率随原子间距变化的趋势。另外,激光脉冲的持续作用可以增强分子的电离,取原子个数为5,基频光波长为800 nm,基波与谐波的强度配比为4,频率配比为2,当其作用时间达到75 fs时,电离基本接近饱和。采用外静电场电离模型能够合理地解释这些现象。     

双色激光场中激光强度和脉宽对线性多原子分子离子电离的影响

 利用强激光场电离和离解分子来研究分子激发态的波包结构是强场物理的重要研究方向。利用短时指数传播子对称分割法和快速傅里叶变换技术,数值求解了一维含时Schr-dinger方程,探讨了双色激光场中激光的基波和谐波强度之间的不同配比以及脉宽对线性多原子分子离子电离的影响。理论计算结果表明：基波和谐波的相对相位为π时,尽管随着激光的基波和谐波强度之间配比的变化,电离几率随原子间距变化的趋势基本保持不变,但在一定的激光基波强度下（1.2×10¹³~1.2×10¹⁵ W/cm²),激光基波强度的变化可以明显改变电离几率随原子间距变化的趋势。另外,激光脉冲的持续作用可以增强分子的电离,取原子个数为5,基频光波长为800 nm,基波与谐波的强度配比为4,频率配比为2,当其作用时间达到75 fs时,电离基本接近饱和。采用外静电场电离模型能够合理地解释这些现象。     

Controlling continuum wavepacket interference by two-color laser field in over-the-barrier ionization regime

Continuum wavepacket interference is investigated by numerically solving the time-dependent Schröodinger equation for the interaction of hydrogen atoms with laser fields. The obtained wavepacket evolution indicates that, in the over-the-barrier ionization regime (10¹⁶ W/cm²), the continuum–continuum (CC) interference of ionizing electrons becomes the main process in highorder harmonics generation (HHG), compared with continuum-bound (CB) transition, as reported by Kohler et al. [Phys. Rev. Lett. 105(20), 203902 (2010)].We propose a two-color laser field scheme for controlling the quantum trajectories of ionizing electrons and for extending the CC harmonic energy. As a result, a high energy platform occurs in the HHG spectrum, which entirely originates from the CC harmonics, with a cutoff adjustable by the relative phase of the two-color fields. This provides further understanding of the dynamic feature of atoms and molecules in super intense laser fields and provides an opportunity to image the atomic or molecular potential.     

Enhanced ionization of vibrational hot carbon disulfide molecules in strong femtosecond laser fields

By using a heated molecular beam in combination with a time-of-flight mass spectrometer, we experimentally study the ionization of vibrational-hot carbon disulfide(CS_2) molecules irradiated by a linearly polarized 800-nm 50-fs strong laser field. The ion yields are measured in a laser intensity range of 7.0 × 10~(12) W/cm~2–1.5 × 10~(14) W/cm~2 at different molecular temperatures of up to 1400 K. Enhanced ionization yield is observed for vibrationally excited CS_2 molecules.The results show that the enhancement decreases as the laser intensity increases, and exhibits non-monotonical dependence on the molecular temperature. According to the calculated potential energy curves of the neutral and ionic electronic states of CS_2, as well as the theoretical models of molecular strong-field ionization available in the literature, we discuss the mechanism of the enhanced ionization of vibrational-hot molecules. It is indicated that the enhanced ionization could be attributed to both the reduced ionization potential with vibrational excitation and the Frank–Condon factors between the neutral and ionic electronic states. Our study paves the way to understanding the effect of nuclear motion on the strongfield ionization of molecules, which would give a further insight into theoretical and experimental investigations on the interaction of polyatomic molecules with strong laser fields.     

超快强激光驱动的原子分子电离

强场电离是超快强激光与物质相互作用时发生的基本物理过程。强场驱动原子分子的电离电子动力学过程发生在一个光学振荡周期以内,是在阿秒时间尺度上研究电子超快动力学的典范。不仅如此,强场驱动下的超短电子束还为探测原子分子的结构及其超快动力学提供了重要的技术手段。文章首先简要阐述了超快强光场中原子分子电离的基本物理图像,在此基础上,介绍了近年来基于强场电离电子开展的超快过程研究的几个例子,最后简要讨论了强场电离研究的未来可能发展方向。     

Atomic ionization by ultra—strong laser fields

The problem of multi-photon ionization of hydrogen by ultra-strong electromagnetic fields is solved in the limit where the field energy is greater than the Coulomb energy. The transition rate goes to zero as the reciprocal of the field strength.