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.     

High-order harmonic generation of pulses with multiple timescales: selection rules,carrier envelope phase and cutoff energy

ABSTRACT

High harmonic generation (HHG) is sensitive to the carrier envelope phase (CEP) of its driving laser field if it is a sufficiently short pulse (several-cycle pulse). Here we show that strong CEP effects can also be found in HHG from long duration multi-cycle pulses (up to 200?fs at 800?nm central wavelength). We find that HHG from multi-cycle pulses may be CEP dependent when the driving pulse exhibits two distinct timescales (multi-timescale pulse): (i) a short timescale associated with the average frequency, and (ii) a long timescale associated with the pulse’s temporal periodicity. The interplay of these timescales results in significant changes to both the cutoff frequency, and the appearance of symmetry allowed harmonics in the spectrum as function of CEP, similar to HHG from several-cycle pulses. We relate this effect to the multi-timescale intensity variations in the driving pulse, and construct an analytical condition to access the phenomenon. Lastly, we numerically demonstrate reconstruction of the CEP through HHG from long duration multi-timescale pulses. Our work may be useful in several areas of strong-field physics and attosecond science, for example, allowing spectroscopy of multi-timescale processes (e.g. HHG from vibrationally active media), and paving the way towards CEP characterisation using long pulses.     

Attosecond spectroscopy for filming the ultrafast movies of atoms,molecules and solids

Three decades ago, a highly nonlinear nonpertubative phenomenon, now well-known as the high harmonic generation (HHG), was discovered when intense laser irradiates gaseous atoms. As the HHG produces broadband coherent radiation, it becomes the most promising source to obtain attosecond pulses. The door to the attosecond science was opened ever since. In this review, we will revisit the incredible adventure to the attoworld. Firstly, the progress of attosecond pulse generation is outlined. Then, we introduce the efforts on imaging the structures or filming the ultrafast dynamics of nuclei and electrons with unprecedented attosecond temporal and Angstrom spatial resolutions, utilizing the obtained attosecond pulses as well as the high harmonic spectrum itself.     

Relativistic laser plasmas for novel radiation sources

Relativistic laser-plasma interaction results in new sources of short-pulsed x-ray radiation. Here we consider two options. The first one is betatron radiation of electrons accelerated in underdense plasmas and oscillating in transverse fields of the laser wake. This radiation is incoherent and broadband, the pulse duration is comparable with that of the driving laser. The second option is the high harmonic generation (HHG) from overdense plasma surfaces. This radiation is coherent. The relativistic high harmonics are phase locked and emerge in the form of (sub-)attosecond pulses. One- and three-dimensional regimes of relativistic HHG from overdense plasmas are considered.     

High-order harmonics generation by few-cycle and multi-cycle femtosecond laser pulses

This paper investigates experimentally high-order harmonic generation(HHG) of neon gas with 5-fs and 25-fs driving laser pulses.It has been demonstrated that the cutoff energy of the harmonic extreme ultraviolet photons is extended to 131 eV and the HHG spectrum near the cutoff region becomes continuum as the driving laser pulse duration is 5 fs;whereas much lower cutoff photon energy and discrete harmonic spectrum near the cutoff region are presented as the laser pulse duration is 25 fs.The results can be explained by the fact that neutral atoms can be exposed to more intense laser field before they are depleted by ionization because of the extremely short rising time of the few-cycle pulse.The 5-fs driving laser pulse paves the way of generation of coherent x-ray in the water window and single attosecond pulse.     

Control mechanism of atomic ionization and high-order harmonic generation assisted by attosecond pulses

Attosecond pulses combined with infrared laser constitute a powerful tool for controlling atomic photoionization and high-order harmonic generation (HHG). We apply the intense-field many-body S-matrix theory to solve such two-pulse excitation problems. The theory can give a clear explanation for the oscillation of ionization probability as a function of time delay between infrared field and attosecond pulses with central frequency lying below ionization threshold at moderate infrared intensities. The HHG assisted by such attosecond pulses is also interpreted. In addition to a known dramatic enhancement of HHG, a harmonic emission from rapid oscillation of bound-state population caused by the counter-rotating wave is presented.     

红外激光场中共振结构原子对极紫外光脉冲的压缩效应

通过数值求解一维原子的含时薛定谔方程, 研究了具有共振结构的原子在双色场(红外激光(IR)+极紫外光(XUV)) 驱动下发射高次谐波的特征. 研究结果表明, 具有共振结构的原子所发射的高次谐波与无共振结构原子(简称为一般原子)发射的高次谐波有明显不同, 共振结构的原子除了在某一能量附近(原子的共振能量+电离能)高次谐波的强度有很大提高外, 它还对XUV光的响应较一般原子表现得更为敏感, 即使XUV光的强度较弱, 也能够明显提高XUV光脉冲中心频率附近的谐波强度, 更重要的是通过调节双色场的时间延迟, 能使输入的XUV光的脉宽得到明显的压缩, 通过时间-频率分析给出了发生这种现象的原因. 由此提出了通过滤波-连续反馈的方式可使XUV光的脉冲从200 as压缩至120 as左右.     

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.     

Probing subcycle spectral structures and dynamics of high-order harmonic generation in crystals

Subcycle spectral structures and dynamics of high-order harmonic generation (HHG) processes of atoms and molecules driven by intense laser fields on the attosecond time scale have been originally studied theoretically and experimentally. However, the time scale of HHG dynamics in crystals is in the order of sub-femtosecond, and the carrier dynamics of HHG in crystals driven by subcycle laser pulses are largely unexplored. Here we perform a theoretical study of subcycle structures, spectra, and dynamics of HHG of crystals in mid-infrared laser fields subject to excitation by a subcycle laser pulse with a time delay. The HHG spectra as a function of time delay between two laser fields are calculated by using a single-band model for the intra-band carrier dynamics in crystal momentum space and by solving the time-dependent Schrödinger equation in velocity gauge for the treatment of multi-band crystal systems. The results exhibit a complex time-delay-dependent oscillatory pattern, and the enhancement and suppression of the HHG related to subcycle pulse are observed at the given time delay in either single-band or multi-band crystal systems. To understand oscillation structures with respect to the dependence for the subcycle laser fields, the time-frequency characteristics of the HHG as well as the probability density distribution of the radiation are analyzed in detail.     

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.     

极化门控制下中红外激光场驱动He原子产生的单个阿秒脉冲

由中红外激光场(波长为2128nm)驱动He原子,在极化门的控制下,通过强场近似方法(SFA)研究了He原子发射高次谐波的特点.研究表明,在这种组合场驱动下He原子可产生截止位置很高的高次谐波,并且在接近截止位置的平台区展现了超连续的特点,对该超连续部分的高次谐波进行叠加,可得到宽度为44.5as的单个超短脉冲.为了了解该超短阿秒脉冲的产生机理,我们对高次谐波谱的发射过程进行了时频分析,分析表明由于极化门的存在,有效地抑制了极化门以外的阿秒脉冲的发射,从而获得单个阿秒脉冲.     

Generation of isolated attosecond pulses with a specific waveform two-color laser field

We theoretically propose a new method for generating intense isolated attosecond pulses during high-order harmonic generation (HHG) process by accurately controlling electron motion with a two-color laser field,which consists of an 800-nm,4-fs elliptically polarized laser field and a 1400-nm,～43-fs linearly polarized laser field.With this method,the supercontinua with a spectral width above 200 eV are obtained,which can support a ～15-as isolated pulse after phase compensation.Classical and quantum analyses explain the controlling effects well.In particular,when the pulse duration of the 800-nm laser field increases to 20-fs,sub-100-as isolated pulses can be obtained even without any phase compensation.     

强激光等离子体相互作用驱动高次谐波与阿秒辐射研究进展

对超快过程的探测和控制决定了人类在微观层面认识和改造物质世界的能力.阿秒光源可完成对组成物质的电子运动及其关联效应进行超高时空分辨的探测和操控,为人类认识微观世界提供了全新手段,被认为是激光科学史上最重要的里程碑之一.世界主要科技强国都将阿秒科学列为未来10年重要的科技发展方向.利用强激光与物质相互作用产生高次谐波是突破飞秒极限实现高亮度阿秒脉冲辐射的重要方案之一,成为了近年来激光等离子体领域的研究热点.本文聚焦强激光与等离子体相互作用中的高次谐波和阿秒脉冲辐射,主要介绍其产生机制、研究进展和前沿应用,并对未来的发展趋势和创新突破进行展望.     

极化门控制下中红外激光场驱动He原子产生的单个阿秒脉冲

由中红外激光场（波长为2128nm）驱动He原子,在极化门的控制下,通过强场近似方法(SFA)研究了He原子发射高次谐波的特点.研究表明,在这种组合场驱动下He原子可产生截止位置很高的高次谐波,并且在接近截止位置的平台区展现了超连续的特点,对该超连续部分的高次谐波进行叠加,可得到宽度为44.5as的单个超短脉冲．为了了解该超短阿秒脉冲的产生机理,我们对高次谐波谱的发射过程进行了时频分析,分析表明由于极化门的存在,有效地抑制了极化门以外的阿秒脉冲的发射,从而获得单个阿秒脉冲．     

线偏振激光场中分子高次谐波椭偏率的调控

高次谐波椭偏率的调控为人们研究磁性材料和手性介质中的超快动力学过程提供了有效途径.本文理论研究了线偏振激光脉冲驱动下,H₂~+和H₃²⁺分子高次谐波的偏振特性及阿秒脉冲产生.结果表明当取向角为0~o时,H₂~+分子谐波的椭偏率几乎为0,而H₃²⁺分子谐波具有较大椭偏率,这是由于分子轨道对称性决定的.通过改变取向角的大小,可以调控高次谐波强度以及谐波椭偏率大小,为产生椭偏XUV脉冲提供了手段.同时,发现椭偏率较大的谐波阶次对应的谐波强度较小,分析表明分子的双中心干涉效应对椭偏率有很大的影响.对于H₂~+和H₃²⁺分子,分别合成了椭偏率为0.75和0.55的椭圆偏振阿秒脉冲.这种大椭偏XUV脉冲的产生为高次谐波在材料与生物科学领域提供了重要应用.     

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     

利用阿秒激光追踪和控制原子分子内部电子的运动(英文)

随着强激光技术的快速发展,在物质与激光相互作用下,实验上发现了很多新奇的物理现象。这些现象成功地被各种理论模型和数值模拟所解释和证明。一种很重要的现象就是所谓的高次谐波产生:在原子和分子与强激光相互作用时,能够放出能量为基频光子能量几倍到几百倍的大能量光子。在实验上,人们已经可以通过合成截止频率附近的几个谐波来产生脉冲长度在阿秒量级的激光脉冲(1阿秒=10~(-18)s)。阿秒脉冲的获得开启了超快科学一个全新的领域:人们可以在电子运动的自然时间尺度上去探测和操控原子分子内部电子的运动,这是继飞秒科学后人们操控微观世界物质运动的又一大飞跃。在本文中,我们就最近几年我们在理论上所开展的阿秒物理做一个简单的综述,重点强调利用阿秒光去控制电子的电离动力学以及探测分子内部电子运动。     

利用阿秒激光追踪和控制原子分子内部电子的运动

随着强激光技术的快速发展, 在物质与激光相互作用下,实验上发现了很多新奇的物理现象。这些现象成功地被各种理论模型和数值模拟所解释和证明。一种很重要的现象就是所谓的高次谐波产生：在原子和分子与强激光相互作用时, 能够放出能量为基频光子能量几倍到几百倍的大能量光子。在实验上, 人们已经可以通过合成截止频率附近的几个谐波来产生脉冲长度在阿秒量级的激光脉冲（1阿秒=10-18秒）。阿秒脉冲的获得开启了超快科学一个全新的领域：人们可以在电子运动的自然时间尺度上去探测和操控原子分子内部电子的运动,这是继飞秒科学后人们操控微观世界物质运动的又一大飞跃。在本文中,我们就最近几年我们在理论上所开展的阿秒物理做一个简单的综述,重点强调利用阿秒光去控制电子的电离动力学以及探测分子内部电子运动.     

Intense ke V IAP generation by orthogonally polarized multicycle midinfrared two-color laser fields

We theoretically investigate the attosecond pulse generation in an orthogonal multicycle midinfrared two-color laser field. It is demonstrated that multiple continuum-like humps, which consist of about twenty orders of harmonics and an intensity of about one order higher than the adjacent normal harmonics, are generated when longer wavelength driving fields are used. By filtering these humps, intense isolated attosecond pulses(IAPs) are directly generated without any phase compensation. Our proposal provides a simple technique to generate intense IAPs with various central photon energies covering the multi-ke V spectral regime by using multicycle midinfrared driving pulses with high pump energy in the experiment.     

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.