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.     

圆偏振激光脉冲附加静电场或太赫兹场时H2+高次谐波产生

本文通过数值求解二维含时薛定谔方程理论的研究了圆偏振激光脉冲(circularly polarized laser pulse, CPLP)作用下H2+的高次谐波产生(high-order harmonic generation, HHG)。通过对比CPLP附加静电场和CPLP附加太赫兹场(terahertz, THz)时的高次谐波发射谱发现,当在CPLP的方向附加静电场时,谐波谱出现双平台结构,且布满调制,通过电子波包概率分布图像发现,电子三次与母核复合,量子轨道之间产生了较严重的干涉。当附加相同强度的THz场时,电子仅两次与母核复合,量子轨道之间的干涉减少,最终得到了86eV到208eV带宽为122eV的连续谱,相比于附加静电场,谐波谱变得连续且平滑,实现了量子轨道调控。最后,利用半经典三步模型、时频分析和电离几率等对谐波发射物理机制进行了深入研究。     

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.     

Generation of elliptical isolated attosecond pulse from oriented H2+ in a linearly polarized laser field

We investigate the ellipticity of the high-order harmonic generation from the oriented H₂⁺ exposed to a linearly polarized laser field by numerically solving the two-dimensional time-dependent Schrödinger equation (2D TDSE). Numerical simulations show that the harmonic ellipticity is remarkably sensitive to the alignment angle. The harmonic spectrum is highly elliptically polarized at a specific alignment angle θ=30°, which is insensitive to the variation of the laser parameters. The position of the harmonic intensity minima indicates the high ellipticity, which can be attributed to the two-center interference effect. The high ellipticity can be explained by the phase difference of the harmonics. This result facilitates the synthesis of a highly elliptical isolated attosecond pulse with duration down to 65 as, which can be served as a powerful tool to explore the ultrafast dynamics of molecules and study chiral light-matter interaction.     

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.     

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.     

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.     

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.     

Controlling the contributions to high-order harmonic generation from different nuclei of N_2 with an orthogonally polarized two-color laser field

The generation of high-order harmonic and the attosecond pulse of the N2 molecule with an orthogonally polarized two-color laser field are investigated by the strong-field Lewenstein model.We show that the control of contributions to high-order harmonic generation(HHG) from different nuclei is realized by properly selecting the relative phase.When the relative phase is chosen to be φ= 0.4π,the contribution to HHG from one nucleus is much more than that from another.Interference between two nuclei can be suppressed greatly; a supercontinuum spectrum of HHG appears from 40 e V to125 e V.The underlying physical mechanism is well explained by the time–frequency analysis and the semi-classical threestep model with a finite initial transverse velocity.By superposing several orders of harmonics,an isolated attosecond pulse with a duration of 80 as can be generated.     

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.     

Minimum structure of high-harmonic spectrafrom aligned O2 and N2 molecules

We experimentally investigated the high-order harmonic generation (HHG) from aligned O₂ and N₂ molecules in a linearly polarized laser field, and presented the dependence of the harmonic spectrum on the driving laser intensity and molecular alignment angle. The minimum position of HHG of O₂ varies with changing the laser intensity, which is caused by multi-orbital interference. However, the location of the observed minimum structure in N₂ harmonic spectrum remained unchanged upon changing the laser intensity. The mechanism of the spectral minimum for N₂ case is regarded as a Cooper-like minimum in HHG associated with the molecular electronic structure. This work indicates that harmonic spectroscopy can effectively uncover information about molecular structure and electron dynamics.     

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.     

双色激光场中高次谐波转化效率的提高

采用渐近边界条件和辛算法数值求解双色激光场与模型P?schl-Teller势相互作用的含时Schr?dinger方程，计算了电离概率、平均位移、高次谐波以及跃迁概率；数值结果显示添加6倍频光的双色激光场能使高次谐波转化效率明显提高.分析了双色激光场极大地提高高次谐波转化效率的机理，并且通过对产生特定级次谐波的跃迁概率的计算，给出高次谐波转化效率提高的具体数值. 关键词： 渐近边界条件 辛算法 双色激光场 高次谐波     

Harmonic emission spectra and attosecond pulse generation from helium atom driven by the mid-infrared nonhomogeneous field

The generations of the high-order harmonics and the attosecond pulses from helium atom driven by the mid-infrared symmetric and asymmetric nonhomogeneous field have been theoretically investigated. It is found that (i) due to the surface plasmon polaritons in the metallic nanostructure, the extensions of the harmonics from the positive and the negative laser amplitudes, or only from the positive laser amplitude can be found for the cases of symmetric and asymmetric nonhomogeneous fields, respectively. (ii) The wavelength scalings of the harmonic cutoff and the harmonic yield show that the harmonic cutoff and the harmonic yield can be extended and decreased with the increase in laser wavelength, respectively. However, due to the limit of the gap size of the nanostructure, the threshold value of the harmonic cutoff can be achieved for a given gap size of the nanostructure. (iii) By adding a weak terahertz field to the mid-infrared fundamental field with the asymmetric nonhomogeneous effect, the intensity of the harmonic plateau can be enhanced by one order of magnitude, showing a 1280?eV supercontinuum with the single quantum trajectory contribution. Finally, by properly superposing the harmonics, some attosecond X-ray pulses shorter than 35 as can be produced.     

Generation of an isolated sub-30 attosecond pulse in a two-color laser field and a static electric field

We theoretically investigate high-order harmonic generation(HHG) from a helium ion model in a two-color laser field,which is synthesized by a fundamental pulse and its second harmonic pulse.It is shown that a supercontinuum spectrum can be generated in the two-color field.However,the spectral intensity is very low,limiting the application of the generated attosecond(as) pulse.By adding a static electric field to the synthesized two-color field,not only is the ionization yield of electrons contributing to the harmonic emission remarkably increased,but also the quantum paths of the HHG can be significantly modulated.As a result,the extension and enhancement of the supercontinuum spectrum are achieved,producing an intense isolated 26-as pulse with a bandwidth of about 170.5 eV.In particular,we also analyse the influence of the laser parameters on the ultrabroad supercontinuum spectrum and isolated sub-30-as pulse generation.     

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.     

Carrier envelope phase effect on the spatial distribution of high-order harmonic generation in asymmetric molecule

The spatial distribution in high-order harmonic generation(HHG) from the asymmetric diatomic molecule He H~(2+) is investigated by numerically solving the non-Born–Oppenheimer time-dependent Schr?dinger equation(TDSE). The spatial distribution of the HHG spectra shows that there is little contribution in HHG around the geometric center of two nuclei(z = 1.17 a.u.) and the equilibrium internuclear position of the H nucleus(z = 3.11 a.u.). We demonstrate the carrier envelope phase(CEP) effect on the spatial distribution of HHG in a few-cycle laser pulse. The HHG process is investigated by the time evolution of the electronic density distribution. The time–frequency analysis of HHG from two nuclei in HeH~(2+) is presented to further explain the underlying physical mechanism.     

基于光场离化电流机制产生强太赫兹辐射的参数优化研究

基于超短激光脉冲与气体作用通过光场离化电流产生太赫兹(THz)辐射的模型, 研究了用双色激光脉冲的方法产生强THz辐射的优化参数条件. 数值计算表明, 导致THz辐射产生的离化电流主要是由一阶电离过程产生的, 高阶离化对该电流产生的贡献很小. 通过调节基频光与倍频光的配比、相位差都能增大离化电流, 从而可以提高THz辐射振幅. 将激光波长拓展到中红外波段, 也有利于提高离化电流. 此外,改变作用气体的种类也能改变离化电流. 在激光和密度参数相等的情况下, 在氦气中可以产生高于氮气中2倍左右的离化电流.     

Frequency dependence of quantum path interference in non-collinear high-order harmonic generation

High-order harmonic generation(HHG) driven by two non-collinear beams including a fundamental and its weak second harmonic is numerically studied. The interference of harmonics from adjacent electron quantum paths is found to be dependent on the relative delay of the driving pulse, and the dependences are different for different harmonic orders.This frequency dependence of the interference is attributed to the spatial frequency chirp in the HHG beam resulting from the harmonic dipole phase, which in turn provides a potential way to gain an insight into the generation of high-order harmonics. As an example, the intensity dependent dipole phase coefficient α is retrieved from the interference fringe.     

Optical high harmonic generation in C60

High harmonic generation (HHG) requires a strong laser field, but in C60 a relatively weak laser field is sufficient. Numerical results presented here show that, while its low order harmonics result from the laser field, its high order ones are mainly from the multiple excitations. Since high order harmonics directly correlate with electronic transitions, the HHG spectrum accurately measures transition energies. Therefore, C60 is not only a promising material for HHG, but may also present an opportunity to develop HHG into an electronic structure probing tool.