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.     

空间非均匀啁啾双色场驱动下氦离子的高次谐波以及孤立阿秒脉冲的产生

本文理论上研究了初态为基态与第一激发态等权叠加的一维氦离子在空间非均匀啁啾双色场驱动下氦离子的高次谐波发射及孤立阿秒脉冲的产生. 研究表明, 一维氦离子在空间非均匀啁啾双色场驱动下发射的高次谐波相对于均匀场情况截止位置得到明显扩展, 得到了光滑的超连续谱,并应用半经典三步模型解释了高次谐波发射的物理机理. 通过小波变换的方法对连续谱进行了时频分析, 并且与电子的经典运动轨迹进行了对比分析, 结果显示在空间非均匀场中长量子轨道消失, 短量子轨道加强. 讨论了空间非均匀啁啾双色场中时间延迟对谐波和孤立阿秒脉冲产生的影响, 发现适当调整时间延迟值可以得到较大延展的光滑的超连续谐波谱, 本方案中时间延迟为t₀=1.6πup/ω₁时得到了最大延展, 通过对谐波中600次到680次(80次)谐波合成得到32 as的孤立脉冲.     

非均匀激光场中氢分子离子高次谐波的增强

通过数值求解非波恩-奥本海默近似下的一维含时薛定谔方程,研究了蝴蝶结型纳米结构基元中氢分子离子高次谐波的产生.研究表明,在蝴蝶结型纳米结构基元内部产生的非均匀场的空间位置对高次谐波的发射有较大影响.当非均匀场的空间位置从30 a.u.平移到-30 a.u.时,高次谐波的截止位置被延展且形成光滑的超连续的谐波谱,并应用时频分析方法、经典三步模型以及电离概率等解释了高次谐波发射的物理机理.研究了高次谐波谱对非均匀场空间位置的依赖性与载波包络值的关系,发现随着载波包络值的变化,非均匀场在不同空间位置处的高次谐波谱变化趋势相同.     

正交偏振双色激光场作用下高次谐波的椭偏特性研究

通过数值求解二维含时薛定谔方程，理论研究了正交偏振双色激光场作用下H2+分子高次谐波发射和孤立阿秒脉冲的产生. 数值结果显示，改变激光场的强度比，可以调控高次谐波强度以及谐波椭偏率. 结果表明随着场强比的增加，y方向的谐波强度不断提高. 当场强比为1:2.5时，x方向和y方向分别仅有奇次谐波和偶次谐波产生，并且偶次谐波的强度比奇次谐波强度高2-3个数量级. 此时，奇次谐波的椭偏率最大可以达到0.3，偶次谐波的椭偏率接近于0. 此外，通过改变分子的准直角可以控制谐波的椭偏率，基于这一现象，利用椭圆偏振高次谐波的平台区合成了椭偏率为0.05的椭圆偏振阿秒脉冲链.     

Exploration of High-Harmonic Generation from the CS_2 Molecule by the Lewenstein Method in Two-Color Circularly Polarized Laser Field

The high harmonic generation(HHG) from the CS_2 molecule in intense laser fields is investigated using the extended Lewenstein method. The initial state is the highest-occupied molecular orbital of the CS_2 molecule,which can be well described by Gaussian wave packet using GAMESS-UK package. Compared with the case of the elliptical laser, the HHG can be extended in two-color circularly polarized laser field. The time-frequency analysis and classical electron trajectory as well as the ionization yield curve are also presented to further explain the underlying mechanism. After adding a static electric field on the z-direction, the single quantum path control is realized and the supercontinuum spectra are obtained. Moreover,an isolated 110 as pulse can be obtained by superposing the harmonics from 130 th to 180 th order.     

利用43飞秒的强激光脉冲实现单个阿秒脉冲输出的新机理

研究了多个光周期的长脉冲(43 fs)激光与氖原子相互作用产生的高次谐波的辐射特性. 通过计算机数值模拟，发现当激光场的强度超过饱和光强时，原子将会在几个光周期内被迅速电离，使得原子的高次谐波谱在截止区呈现出平滑的多平台结构. 同时，在高频波段离子产生的高次谐波的影响将变得十分显著. 通过选取合适的子平台进行频率叠加，在消除了离子的高次谐波的影响后，可以获得单个的阿秒软X射线脉冲. 关键词： 高次谐波 阿秒脉冲     

双色激光脉冲相位差对晶体发射高次谐波 的影响

通过数值求解双色激光场(基频场和二倍频场)与一维晶体相互作用的含时薛定谔方程,研究了晶体在双色激光脉冲驱动下发射高次谐波的特点.研究结果表明,晶体在双色激光脉冲驱动下发射的高次谐波第二平台强度相对于单色激光脉冲驱动下有显著提高,且随双色激光脉冲的相位差明显变化.进一步的研究发现,在双色激光脉冲其它参数保持不变的情况下,通过调节双色激光脉冲的相位差就能有效提高晶体发射高次谐波第二平台的产额,提高的幅度会随激光脉冲的宽度有所不同.     

不同取向角下CO2分子波长依赖的垂直谐波效率

通过数值计算, 研究了强激光场中CO₂ 分子在不同波长和取向角下产生的高次谐波辐射的效率. 发现CO₂ 分子的垂直谐波效率在较小的和中间的取向角时倾向于与平行谐波效率可比或更高, 而在较大的取向角时, 垂直谐波效率远低于平行谐波效率. 进一步的分析表明, CO₂ 分子的结构对其垂直谐波效率有重要的影响, 且该影响与波长有关. 建议对于较复杂的分子, 应该在分子的轨道成像实验中考虑垂直谐波的贡献.     

Higher harmonic generation in laser plasma upon interaction of femtosecond laser pulses with doubly and singly charged ions under conditions of resonance frequency conversion of laser radiation

The higher harmonic generation (HHG) in plasmas formed on the surface of different solid targets (Pb, Ag, Ge, In, Au, Cr, Pt, V, Mn, Ga, Bi, Sb, Cu, Al, Ca, and Sn) by laser ablation is studied. The possibility of HHG upon interaction of femtosecond radiation with doubly charged ions is studied on the example of Mn plasma. This process allowed generation of higher harmonics of up to the 101st order. The results of investigation of individual enhanced harmonics in Sn, Sb, In, and Cr plasmas are presented. Comparison of the conditions of HHG in weakly and strongly excited plasmas showed that the latter is preferable for efficient frequency conversion. It is demonstrated that the use of laser plasma spectroscopy with high time resolution allows one to determine the optimal conditions for generation of harmonics with a plateaulike distribution in the far-UV spectral region.     

Extending the High-Order Harmonics Plateau and Isolated Attosecond Pulse Generation in an Intense Three-Color Laser Field

We propose a method to extend the high-order harmonics plateau and generate an isolated sub-10-as pulse by adding a weak control pulse (10 fs, 1600 nm) to modify a two-color laser field (5 fs, 800 nm; 10 fs, 400 nm). The numerical results show that the plateau is extended obviously in the three-color laser field regime. Additionally, the ionization rate and classical returning kinetic-energy maps are calculated to better understand the physical origin of the high-order harmonics generation (HHG). By means of the ionization probability and the time-frequency distributions, more features of the HHG are revealed. Furthermore, our simulations show that the width of the plateau and the relative conversion efficiency of the harmonic spectra are highly dependent on the relative phase. Finally, by adjusting the relative phase and superposing a properly selected range of the HHG spectrum, an isolated attosecond pulse with a duration of 7 as is obtained.     

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.     

激光强度依赖的阈下谐波产生机制

利用广义伪谱方法精确数值求解了氢原子在强激光场中的三维含时薛定谔方程,获得了强激光中氢原子的含时波函数,利用时间依赖的偶极矩的傅里叶变换得到了高次谐波谱,研究了氢原子在强激光场中发射低于电离阈值的谐波谱对激光强度的依赖性.研究发现,激光强度在低于电离阈值的谐波产生的通道选择的过程中扮演着重要角色,主要有两种量子通道对阈下谐波的产生有贡献,即广义的短轨道和长轨道,其中长轨道对激光场强度比较敏感.结合小波时频变换、经典轨道分析、以及强度依赖的量子通道选择分析,本文阐明了其背后的物理机制.     

Interference and spectral broadening of higher harmonics of laser radiation in plasma torches containing ions,nanoparticles, and fullerenes

We analyze the interference between two processes of higher harmonic generation (HHG) in plasma containing mixtures of different materials (silver and gold nanoparticles, as well as graphite and boron). We find that, for mixtures and individual ingredients, the limiting orders of generated harmonics of laser radiation approximately coincide with one another. At the same time, for plasma torches formed by the ablation of mixtures of materials, the HHG efficiency is considerably reduced compared to the case of the frequency transformation of laser radiation in individual ingredients of these mixtures as a result of destructive interference in the former case. We demonstrate a considerable spectral broadening of harmonics generated in laser plasma with pulses passed through filaments formed in air. In this case, the HHG efficiency increases fourfold (from 3 × 10⁻⁶ to 1.2 × 10⁻⁵) compared to the case of radiation free of phase and frequency modulation. The generation of harmonics is also observed upon the passage of 120-fs laser pulses through plasma containing fullerenes. In this case, the limiting value of generated harmonics achieves the 33rd order. The efficiency of harmonics in fullerene plasma considerably exceeds a similar process in silver plasma.     

Generation of higher harmonics of laser radiation in plasma formed by pulses with a 1-kHz repetition rate

Studies of higher-order nonlinearities in plasma plumes by the method of higher-harmonic generation (HHG) upon laser ablation of different materials by pulses with a repetition rate of 1 kHz are reviewed. It is shown that an increase in the pulse repetition rate compared to the previous works on HHG in plasma using lasers with a pulse repetition rate of 10 KHz considerably increases the average power of converted radiation in the far-ultraviolet (FUV) region. The review considers the results of works on the interference of quantum trajectories of accelerated electrons, two-color pumping, HHG in graphite plasma, HHG in gases compared to HHG in plasma plumes, resonant enhancement of harmonics, and stabilization of the output parameters of radiation converted in plasma. It is shown that the new methods of optimization of the HHG process considerably increase the potential of the use of coherent FUV radiation owing to the improvement of some characteristics of harmonics in plasma generated by pulses with a high repetition rate.     

利用三色组合脉冲激光获得孤立阿秒脉冲发射

孤立阿秒脉冲因可以跟踪和控制原子及分子内电子的运动过程而备受关注.本文从理论上开展了氦原子在3束飞秒脉冲激光组合场辐照下产生的高次谐波和阿秒脉冲辐射的研究.组合激光场由16 fs/1600 nm,15 fs/1100 nm和5.3 fs/800 nm的钛宝石脉冲构成.与前两束脉冲合成的双色场产生谐波谱相比,附加钛宝石脉冲的三色场产生的高次谐波发射谱呈现出高转换效率及宽带超连续特性,超连续谱范围覆盖从230—690次谐波,傅里叶变换后实现了128 as高强度孤立短脉冲的产生.该结果归因于合成的三色场呈现出高功率及少周期的中红外飞秒脉冲激光特性,可以有效控制原子电离以及复合发生在中红外飞秒脉冲的一个有效光学周期内.     

High field physics and extreme nonlinear optics

Despite the fact that high order harmonic generation (HHG) aims at serving as a table-top light source for imaging applications with extremely high spatial resolution, a general lack of accurate conversion efficiency measurements exists in the field. Here, we present such a measurement for a HHG setup with a semi-infinite gas cell. By combining measurements with a calibrated photodiode sensitive in the extreme ultra-violet (XUV) and spatially resolved spectral measurements of HHG spectra, we are able to determine conversion efficiencies of the HHG process as well as brilliance values for individual harmonics. The method is explained in detail and applicable to any target geometry.     

少周期激光脉冲附加太赫兹场对高次谐波发射的影响

本文通过数值求解非伯恩奥本海默近似下电子一维核一维的含时薛定谔方程,研究了少周期线偏振激光与氢分子离子相互作用下,太赫兹场的加入对高次谐波的发射影响.我们发现,在短周期线偏振激光脉冲的y方向上附加一个强度较弱的太赫兹场可以有效地扩展谐波的截止位置,并对量子轨道实现调控.通过时频分析、电子波包随时间变化以及半经典三步模型研究了高次谐波发射的物理机制,并对获得的物理现象给出合理的解释.     

等离子体光栅靶的表面粗糙度对高次谐波产生的影响

极紫外光和软X射线由于其波长和脉冲持续时间极短,可用于超快物理过程和物质微观结构的探测.最近几年,研究人员发现激光和等离子体相互作用可以产生持续时间极短(阿秒)且相干性较好的高次谐波辐射,其波长可接近甚至达到水窗波段.然而,实验研究指出,理论上应出现的一些谐波在实验中并没有出现.本文针对超短超强激光与非理想条件下的等离子体光栅靶相互作用产生高次谐波的物理过程进行了理论分析和粒子模拟.研究结果表明,等离子体光栅的周期性结构对于高次谐波的频谱和辐射角分布存在显著调制效果.光栅靶表面粗糙度直接影响光栅的光学调制效果,改变高次谐波的频谱分布和辐射角分布.理想光栅条件下,满足光栅匹配条件的特定阶数谐波明显获得增强,且辐射张角集中在平行靶面的方向.靶表面粗糙度的出现,导致光栅匹配条件失效,高次谐波能量向各阶分散且辐射张角逐渐偏离靶表面方向.研究结果较好地解释了实验中观测到的谐波频谱分布,为进一步的研究提供了一定参考.     

Orientation dependence in high harmonics of ZnO with polarization corrections to counteract the birefringent effect

We investigate the influence of the birefringence on the high-order harmonics in an a-cut Zn O crystal with midinfrared laser pulses. The high harmonics exhibit strong dependence on the alignment of the crystal with respect to the laser polarization. We introduce the Jones calculus to counteract the birefringent effect and obtain the harmonics with polarization corrections in Zn O. We show that the birefringent effect plays an important role in the orientation dependence of HHG.     

Orientation and ellipticity dependence of high-order harmonic generation in nanowires

It has been predicted that high-order harmonic generation (HHG) in nanowires has the potential to scale up photon energy and harmonic yield. However, studies on HHG in nanowires are still theoretical and no relevant experimental results have been reported as yet. Our experimental observation of the high-order harmonic in cadmium sulfide nanowires (CdS NWs) excited by a mid-infrared laser is, to our knowledge, the first of such study, and it verifies some of the theoretical results. Our experimental results show that the observed harmonics are strongest when a pump laser is parallel to the nanowires. Therefore, the theoretical prediction that harmonics are strongest under the nanowires parallel to the laser field is confirmed experimentally, and this can be used to determine the orientation of the nanowire. In addition, harmonics are sensitive to the variation of pump light ellipticities. This orientation dependence opens new opportunities to access the ultrafast and strong-field physics of nanowires.