Decoding the electron dynamics in high-order harmonic generation from asymmetric molecular ions in elliptically polarized laser fields

The high-order harmonic generation from an asymmetric molecular ion is theoretically investigated based on the Born-Oppenheimer model with two-dimensional electron dynamics. It is shown that the harmonic intensity changes periodically in elliptically polarized laser fields. The periodical character is ellipticity-dependent. By establishing the physical image, the periodicity of the harmonic intensity can be ascribed to the contributions of the ground state and the excited state. Furthermore, the electron dynamics from different electronic states can be selected via combining the elliptically polarized laser field with a static electric field. The harmonics dominated either by ground state or excited state are emitted once in an optical cycle in the combined laser field.     

Accurate prediction of interference minima in linear molecular harmonic spectra by a modified two-center model

We demonstrate that the interference minima in the linear molecular harmonic spectra can be accurately predicted by a modified two-center model. Based on systematically investigating the interference minima in the linear molecular harmonic spectra by the strong-field approximation(SFA), it is found that the locations of the harmonic minima are related not only to the nuclear distance between the two main atoms contributing to the harmonic generation, but also to the symmetry of the molecular orbital. Therefore, we modify the initial phase difference between the double wave sources in the two-center model, and predict the harmonic minimum positions consistent with those simulated by SFA.     

New results in above-threshold ionization and high-order harmonic generation of atomic and molecular systems

Numerical results obtained applying the strong-field approximation to atomic and molecular processes in intense laser fields are presented. In particular, the forward-backward asymmetry in high-order above-threshold ionization (HATI) of Ar atoms by a few-cycle laser pulse is considered. It is shown that the resonantlike enhancements observed in the focal-averaged spectra disappear with the decreasing laser pulse duration. For HATI and high-order harmonic generation (HHG) by molecular systems, we present new results for diatomic molecules. The choice of gauge and the problem of dressing of the initial bound state are discussed. The appearance of the interference minima in molecular HATI and HHG spectra and their role in the characterization of the molecular structure are considered using the example of the Ar₂ molecule.     

Multi-photon resonance enhanced super high-order harmonic generation

This paper proposes highly charged ions pumped by intense laser to produce very high order harmonics.Numerical simulations and full quantum theory of Ne 9+ ions driven by laser pulses at 1064 nm in the power range of 10 9 W/cm 2 ～ 10 15 W/cm 2 show that the emission spectrum corresponds to the electronic transitions from the excited states to the ground state,which is very different from the spectrum of general high-order harmonic generation.In such situation,harmonic order as high as 1000 can be obtained without producing lower order harmonics and the energy conversion efficiency is close to general high order harmonic generation of hydrogen atom in the same laser field.     

On the Validity of Several Methods of Calculation of Vibronic Energy Relaxation Rates

Different approximation methods of calculation of the rates of vibronic energy relaxation are studied and compared with an exact one. The molecular vibrations are described by harmonic oscillators, the positions of equilibrium of which are assumed to be different in different electronic states. The finite line widths of the vibronic states are taken into account. It is found that the approximation methods provide too small values of the relaxation rates, particularly as the coupling strength becomes weak.     

理论研究激光强度对H2+分子高次谐波产生的影响

本文通过求解非波恩-奥本海默近似条件下的一维含时薛定谔方程来研究脉冲强度对H₂⁺分子高次谐波的影响.由于干涉相消,在啁啾激光场的条件下在谐波谱中出现了干涉最小值.我们用全量子方法计算的时频分布图分析了分子高次谐波产生中的微观机制.此外,数值计算结果显示随着脉冲强度的增加电子的有质动力势随之增加,同时干涉最小值的位置移向谐波的高阶部分.     

利用三束中红外空间非均匀激光场产生超长平台区

数值研究了氦离子在三束中红外激光场下发射高次谐波以及阿秒脉冲的特点. 计算结果表明, 通过适当调节三束激光场的延迟时间和相位角, 不仅谐波发射的截止能量得到了延伸, 而且单一的量子路径也被选择出来对谐波发射起作用, 随后通过适当的引入空间非均匀参数,谐波截止能量得到了进一步扩展,形成了一个超长的1773eV的平台区. 并且我们发现当选择氦离子的基态和第一激发态为叠加初始态时,谐波的强度被增强了4-6个数量级. 最后, 通过叠加谐波谱上的谐波, 可获得一系列脉宽为32as左右的阿秒X射线光源. 并且这些光源的强度比氦离子基态作为初始态时增强了4-6个数量级.     

利用三束中红外空间非均匀激光场产生超长平台区

数值研究了氦离子在三束中红外激光场下发射高次谐波以及阿秒脉冲的特点. 计算结果表明, 通过适当调节三束激光场的延迟时间和相位角, 不仅谐波发射的截止能量得到了延伸, 而且单一的量子路径也被选择出来对谐波发射起作用, 随后通过适当的引入空间非均匀参数,谐波截止能量得到了进一步扩展,形成了一个超长的1773eV的平台区. 并且我们发现当选择氦离子的基态和第一激发态为叠加初始态时,谐波的强度被增强了4-6个数量级. 最后, 通过叠加谐波谱上的谐波, 可获得一系列脉宽为32as左右的阿秒X射线光源. 并且这些光源的强度比氦离子基态作为初始态时增强了4-6个数量级.     

在双色场中使用相干叠加态来提高高次谐波的发射

本文提出了一种在双色场中使用相干叠加态来提高高次谐波发射效率的方法. 我们首先通过在800nm基本激光脉冲上添加一束控制激光脉冲在理论上得到双色合成激光场;其次,通过求解一维含时薛定谔方程,计算得到了体系处于不同初始态时的高次谐波谱,并结合时频分布图对其微观机理进行分析. 计算结果表明,使用相干叠加态作为体系的初始态,通过调节两束激光的相对相位可以有效实现提高高次谐波的发射效率的目的.     

On the topology of the adiabatic potential energy surfaces of the H2-ion in a strong magnetic field

The electronic structure of diatomic molecules in strong magnetic fields is investigated by means of the example of the hydrogen molecular ion. A variety of different possibilities for the topological behaviour of the two-dimensional adiabatic electronic potential energy surfaces are derived and discussed. Global as well as local equilibrium configurations of the ion are shown to occur not only for the positions with higher symmetry, i.e. for the parallel and perpendicular positions, but also for configurations which correspond to an inclination of the internuclear axis with respect to the external field.     

在双色场中使用相干叠加态来提高高次谐波的发射

本文提出了一种在双色场中使用相干叠加态来提高高次谐波发射效率的方法.我们首先通过在800 nm基本激光脉冲上添加一束控制激光脉冲在理论上得到双色合成激光场;其次,通过求解一维含时薛定谔方程,计算得到了体系处于不同初始态时的高次谐波谱,并结合时频分布图时其微观机理进行分析.计算结果表明,使用相干叠加态作为体系的初始态,通过调节两束激光的相对相位可以有效实现提高高次谐波的发射效率的目的.     

在不同激光脉宽下的高次谐波

用数值计算方法计算了不同强激光脉冲宽度下高次谐波的产生.我们发现对于激光场强度不高,不能有效电离初态的激光场,长脉冲宽度可以更有效产生高次谐波;而对于高场强的激光场,由于它能够在几个光学周期之内把原子的初态全部电离,所以短脉冲的激光场能够更有效产生高次谐波.     

Theoretical Exploration of the Isotopic Effect on Molecular High-Order Harmonic Generation

The isotopic effect on the generation of the molecular high-order harmonics is studied by numerically solving the one-dimensional time-dependent Schrödinger equation when the model hydrogen molecule ions/hydrogen deuterium molecule ions are exposed to an intense laser pulse. To explain the effect more clearly, not only the ionization probabilities but also the electron–nuclear probability density distributions and time-frequency profiles are calculated. The results show that more intense harmonics are generated in the asymmetric diatomic molecule ions/hydrogen deuterium molecule ions than those of hydrogen molecule ions. Moreover, the interference minimum in the harmonic spectra is investigated by adjusting the laser intensity and the initial vibrational state. It is shown that the interference minimum is sensitive to the laser intensity and the initial vibrational level for hydrogen molecule ions; in contrast, it is only dependent on the initial vibrational level for hydrogen deuterium molecule ions.     

Two-center interference in high-harmonic generation of H_2~+ in a combination of a mid-infrared laser field and a terahertz field

We theoretically investigate the two-center interference in high-order harmonics generated from the H_2~+ in a combination of a mid-infrared laser and a terahertz field by numerically solving the time-dependent Schr ¨odinger equation(TDSE).The interference minima in high-order harmonic generation(HHG) are effectively suppressed when a THz field is added.The contribution to HHG from the two separate nuclei is used to demonstrate the locating order of the harmonic minima.Furthermore, we also investigate the emission time of harmonics. The results show that the intensity of the short path around 60 thorder after adding a THz field is stronger than that in the mid-infrared laser field, which further illustrates the suppression of the interference minima in HHG.     

Theoretical investigation of high-order harmonic generation from asymmetric molecular ions in the chirped laser field

High-order harmonic generation from the asymmetric helium hydrogen molecular ion exposed to a few-cycle chirped laser field is theoretically investigated by numerically solving the reduced one-dimension non-Born–Oppenheimer time dependent Schrödinger equation. The numerical results show that the plateau of the high-order harmonic spectrum is dramatically broadened and smoother with the introduction of the chirp. Further study presents that only the short quantum path contributes to harmonic emission and the long quantum path disappears in the chirped laser. In addition, an 80-as isolated attosecond pulse is obtained by superposing the harmonics from the 100th to the 130th order in the chirped field. The time-frequency distributions and the electronic probability distributions are presented to explain the underlying physical mechanism.     

Ultrahigh Harmonic Generation from an Atom with Superposition of Ground State and Highly Excited States

We investigate the high-order harmonic generation from an atom prepared in a superposition of ground state and highly excited state. When the atom is irradiated by an ultrashort pulse, the cutoff position of the plateau in the harmonic spectrum is largely extended compared with the case that the atom is initially in the ground state. The physics of the extension of the high-order harmonic plateau can be interpreted by the spatial structure of the atomic initial wave packet. We can optimize the generation of high-order harmonics by substituting the excited state for a particular coherent superposition of some highly excited states to form a spatially localized excited wave packet.     

Theoretical investigations of the SH and LiS cations

Reliable theoretical data on spectroscopy and spin-orbit matrix elements are computed for the lowest electronic states of SH⁺ and LiS⁺ ions. Accurate spectroscopic predictions for their excited electronic states are given. For SH⁺, polarization minima at large internuclear distances are located in addition to the strongly bound electronic states already known. For LiS⁺, our calculations confirm that the electronic ground state of this ion is of ³Σ⁻ species and reveal the existence of a ¹Δ state presenting a potential well as deep as the potential of the ground state. Moreover, the LiS⁺ electronic excited states potential energy curves possess shallow potential minima in the molecular region and at long-internuclear distances. Generally, these shallow minima may be populated during low energy collisions between the corresponding atomic fragments. Finally, spin-orbit calculations have allowed giving accurate determinations of the spin-orbit splittings for these cations and elucidation of the predissociation mechanisms of SH⁺ leading to the formation of the S⁺ and H species in their electronic ground states. Accordingly, long-lived SH⁺ ions can be found in the X³Σ⁻, a¹Δ and b¹Σ⁺ electronic states and the rovibrational levels of LiS⁺ in its electronically excited and ground states should be weakly perturbed.     

Molecular recollision interferometry in high harmonic generation

We use extreme-ultraviolet interferometry to measure the phase of high-order harmonic generation from transiently aligned CO(2) molecules. We unambiguously observe a reversal in phase of the high-order harmonic emission for higher harmonic orders with a sufficient degree of alignment. This results from molecular-scale quantum interferences between the molecular electronic wave function and the recolliding electron as it recombines with the molecule, and is consistent with a two-center model. Furthermore, using the combined harmonic intensity and phase information, we extract accurate information on the dispersion relation of the returning electron wave packet as a function of harmonic order. This analysis shows evidence of the effect of the molecular potential on the recolliding electron wave.     

强激光场中模型氢原子和真实氢原子的高次谐波与电离特性研究

利用数值方法求解含时薛定谔方程，研究了一维、二维模型氢原子和真实的三维氢原子在强激光场中产生的高次谐波和电离特性.结果表明，在多光子电离区域和过垒电离区域，模型氢原子与真实的氢原子产生的高次谐波和电离概率差别很小；在隧道电离区域，它们产生的高次谐波的平台特征和截止位置相似，电离概率随时间变化的趋势相近，但其数值有明显的差异.对产生这种差异的原因进行了分析. 关键词： 强激光场 高次谐波 电离概率     

Single Ultrashort Attosecond Pulse Generation via Combination of Chirped Fundamental Laser and an Ultraviolet Controlling Pulse

We theoretically study the high-order harmonic generation (HHG) from a hydrogen atom in an intense few-cycle chirped fundamental laser in combination with an ultraviolet (uv) controlling pulse.The high-order harmonic spectrum is calculated by solving the time-dependent Schr¨odinger equation using the split-operator method.In our calculation,we present the difference of the high-order harmonic spectrum from one-dimensional (1D) model hydrogen atom and three-dimensional (3D) real hydrogen atom.We found that the plateau of the high-order harmonic generation from the 1D case and 3D case are all extended effectively to I p + 35U p due to the presence of the chirped laser pulse and the HHG supercontinuum spectrum is generated by adding an ultraviolet controlling pulse at a proper time,but the efficiency of the HHG for 3D case is more higher at the near cut-off region than the 1D case.Therefore,the generation of the attosecond pulse by synthesizing the harmonics near cut-off region have some slight differences between 1D and 3D simulations.As a real 3D case study,we show that an isolated 18 as pulse with a bandwidth of 232.5 eV is generated directly by optmizing the combination laser fields.