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.     

Amplitude and rotation of the ellipticity of harmonicsfrom a linearly polarized laser field

We simulate the dynamic response of H₂⁺ in a linearly polarized laser field by numerically solving the time-dependent Schrödinger equation. The elliptically polarized high-order harmonics generated by H₂⁺ irradiated by the linearly polarized laser field are systematically investigated. The result shows that the amplitude and rotation of the ellipticity of harmonics are affected by the alignment angle and internuclear distance of the molecule. Analyzing the change in forces acted on the ionized electrons and the trajectories of the electrons, the phenomena are found to be due to the change in the direction of the total Coulomb forces from the two nuclei felt by the recollided ionized electrons in the direction perpendicular to the laser polarization direction. Based on the influence law, we can select the harmonics with a specific frequency band under different alignment angles and then synthesize the isolated attosecond pulses with different rotations, which can be continuously converted from right-handed circular polarization, linear polarization, and left-handed circular polarization by changing the alignment angle. This study provides a new possible approach to the real-time detection of molecular states by using attosecond pulses and obtaining more optimized harmonics with molecular properties.     

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.     

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.     

相对论圆偏振激光与固体靶作用产生高次谐波

超短超强激光与固体靶表面等离子体相互作用可以通过高次谐波的方式产生从极紫外到软X射线波段的相干辐射,获得飞秒甚至阿秒量级的超短脉冲,可用于观测原子或分子中的电子运动等超快动力学过程.本文实验研究了相对论圆偏振飞秒激光与固体靶相互作用的高次谐波产生过程,实验结果表明,在较大入射角下,圆偏振激光也可以有效地产生高次谐波辐射.通过预脉冲控制靶表面的预等离子体密度标长,发现高次谐波的产生效率随密度标长的增加而单调下降.进一步通过二维粒子模拟程序,分析了激光的偏振以及预等离子体密度标长对高次谐波产生的影响,很好地解释了实验观测结果.     

Origin for ellipticity of high-order harmonics generated in atomic gases and the sublaser-cycle evolution of harmonic polarization

We investigate numerically and analytically the polarization properties of high-order harmonics generated by an atom in intense elliptically polarized laser field. The offset angle of the harmonic polarization ellipse can be well described with the semiclassic "simple-man" high-harmonic generation model. The harmonic ellipticity itself, however, can be hardly understood within this model. We show that this ellipticity originates from quantum-mechanical uncertainty of the electron motion. We develop a theoretical approach describing this ellipticity and, more generally, the time evolution of the high-harmonic polarization state within the laser cycle. The analytical results are verified with the exact numerical solution; to make the comparison accurately, we develop a specific technique for separating the contributions of quantum paths in the numerical calculation.     

任意偏振双色相干场高次谐波

系统地研究了任意偏振双色相干场高次谐波，结果表明单个圆偏振光不能产生高次谐波，在适当的条件下，某些谐波可以部分或完全消失，而某些谐波可以得到加强，产生更高次谐波高转换效率的条件是双色线偏振场的结合。     

Elliptic dichroism, ellipticity and the offset angle of high harmonics generated by arbitrary homonuclear diatomic molecules

The nth harmonic emission rate has contributions of the components of the T-matrix element in the direction of the laser-field polarization and in the direction perpendicular to it. Using both components of the T-matrix element we present a theoretical approach for calculation of the ellipticity and the offset angle of high harmonics. The molecular bound state is represented by HOMO or by HOMO-1. We show that high harmonics, generated by molecules oriented by an angle ??_L with respect to the major semiaxis of the laserfield polarization ellipse, are elliptically polarized even if the applied field is linearly polarized. Using examples of N₂ and O₂ molecules we show the existence of extrema and sudden changes of the harmonic ellipticity and the offset angle for particular molecular alignment. The interference between different contributions to the T-matrix element depends on the molecular symmetry. Presenting partial or total parameters of elliptic dichroism in the (??_L, n) plane clear interference minima are observed. Therefore, the measurement of the elliptic dichroism may reveal information about the molecular structure and symmetry.     

Ellipticity dependence of high-order above-threshold ionization from aligned diatomic molecules

We investigate high-order above-threshold ionization of the Ar₂ molecule by an elliptically polarized laser field. In order to describe this process we use the modified molecular strong-field approximation. We have found that the differential ionization rate is a very sensitive function of the ellipticity of the laser field and of the molecular orientation. For parallel orientation the rate has the maximum value for linear polarization, independently of the laser intensity. On the other hand, for perpendicular orientation the rate is maximal for a particular value of the ellipticity which is different from zero. Such a behavior can be related to the molecular symmetry. We consider the differential ionization rate of high-energy electrons as a function of the ellipticity for different internuclear distances. We also present, in the electron energy-emission angle plane, our new results for the focal-averaged spectra of electrons ionized by an elliptically polarized laser field. We have found that, in this case, the two-source two-rescattering-centers interference minima are blurred.     

共振线极化光实现原子矢量磁力仪的理论研究

共振线偏振光激发原子张量磁矩,本文理论研究在矢量磁场和射频场的共同作用下,张量磁矩进动的模型,求解刘维尔方程获得透射光时域完整解析解,包括直流、一次和二次谐波分量.研究发现:当进动的拉比频率Ω1/(22~(1/2))时,两谐波间的干涉效应使直流分量和一次谐波对称成分的单吸收峰劈裂成双峰,裂距((Ω~2+Ω~4-Ω~2-1)~(3/2))~(1/2),一次谐波反对称成分在共振处产生干涉条纹.研究结果显示,谐波间的干涉也可导致直流分量和二次谐波线宽仅为一次谐波线宽的38%,且存在磁场取向临界点,在不同的取向区间分别利用直流及两谐波共振信号辨析磁场变化,可获得最佳测磁灵敏度;同时还可通过共振时直流分量及两谐波对称成分振幅来确定磁场与激光极化方向的夹角,利用两谐波反对称成分相移的差值来确定待测磁场在垂直光极化方向投影与射频场方向的夹角,进而实现结构简单的张量磁矩进动型矢量磁力仪.这种磁力仪适合构成磁力仪阵列,可用于磁定位、水下磁异常源的检测和地磁导航等领域.     

三色圆偏振激光组合脉冲驱动氦原子产生椭圆偏振的阿秒脉冲

我们提出利用频率为ω,3ω和强度较弱的2ω组成的三色圆偏振激光组合脉冲驱动氦原子能够得到椭偏率较大的阿秒脉冲链的一种方法.通过强场近似方法,计算了氦原子在两色和三色圆偏振激光组合脉冲驱动下发射高次谐波谱及其合成阿秒脉冲链,比较了氦原子(初态为s态)在这两种情况下发射高次谐波谱的特点及其合成阿秒脉冲链椭偏率的大小,结果发现,在反旋的两色ω,3ω激光脉冲基础上加入了频率为2ω的第三色激光脉冲联合作用到氦原子上,所得到的阿秒脉冲链的椭偏率相对于双圆场情况下有所增加,通过调整ω,3ω激光的强度比,并且选择适当的第三色激光的强度,对初态为s态的原子,仍能够得到具有较大椭偏率的阿秒脉冲链.     

Investigation of vortex arms in electron vortices by counter-rotating elliptically polarized attosecond laser pulses

We theoretically investigate the vortex patterns in photoelectron momentum distributions of He⁺driven by counter-rotating elliptically polarized,time delayed attosecond laser pulses by numerically solving the two-dimensional time-dependent Schrodinger equation.It is found that the number of vortex arms is extremely sensitive to the ellipticity and wavelength of counterrotating elliptically polarized laser pulses,which is illustrated by the attosecond perturbation ionization models.In addition,the effect of different time delays between two pulses on the interference patterns is also investigated and the corresponding physical mechanism is demonstrated.Since the wavelength,ellipticity and time delay have a significant effect on the vortex interference patterns,this may be a new method for laser field detection.     

任意偏振激光作用下二维模型H原子的谐波发射

采用二维渐近边界条件和辛算法数值求解了任意偏振激光和H原子相互作用的二维含时Schrödinger方程的无穷空间初值问题. 计算了二维H原子在不同偏振激光作用下的谐波发射,得到各种椭圆率下谐波谱的特点与已有文献结果一致.通过电子的基态布居概率和某一时刻的概率密度分布以及电子的平均位移,对不同椭圆率下谐波谱的特点进行了分析. 结果表明,将渐近边界条件和辛算法推广到二维是合理和有效的. 关键词： 二维渐近边界条件 辛算法 任意偏振激光 高次谐波     

Nonsequential double ionization of diatomic molecules by elliptically polarized laser pulses

Using the classical ensemble method, we investigate nonsequential double ionization （NSDI） of diatomic molecules by elliptically polarized laser pulses. The results show that the ellipticity of the laser field has a strong suppression effect on NSDI probabilities both in parallel and perpendicular alignments. The double ionization （DI） channel is commonly dominated by NSDI, and the NSDI channel changes with ellipticity. As ellipticity increases, more and more NSDIs occur through recollision excitation with subsequent field ionization （RESI）. Moreover, like the case of linear polarization, the two electrons involved in NSDI for perpendicularly aligned molecules are more likely to emit into the opposite hemispheres as compared to the case of parallel alignment. Additionally, this alignment effect increases as ellipticity increases.     

High-order harmonic generation of the cyclo[18]carbon molecule irradiated by circularly polarized laser pulse

High-order harmonic generation of the cyclo[18]carbon (C₁₈) molecule under few-cycle circularly polarized laser pulse is studied by time-dependent density functional theory. Compared with the harmonic emission of the ring molecule C₆ H₆ having similar ionization potential, the C₁₈ molecule has higher efficiency and cutoff energy than C₆ H₆ with the same laser field parameters. Further researches indicate that the harmonic efficiency and cutoff energy of the C₁₈ molecule increase gradually with the increase of the laser intensity of the driving laser or decrease of the wavelength, both are larger than those of the C₆ H₆ molecule. Through the analysis of the time-dependent evolution of the electronic wave packets, it is also found that the higher efficiency of harmonic generation can be attributed to the larger spatial scale of the C₁₈ molecule, which leads to a greater chance for the ionized electrons from one atom to recombine with others of the parent molecule. Selecting the suitable driving laser pulse, it is demonstrated that high-order harmonic generation in the C₁₈ molecule has a wide range of applications in producing circularly polarized isolated attosecond pulse.     

Generation of Near-Circularly Polarized Attosecond Pulse with Tunable Helicity by Unidirectionally Rotating Laser Field

A method to produce circularly polarized attosecond pulses with tunable helicity from CO molecule by using an unidirectionally rotating laser field is proposed. It is found that broadband harmonic supercontinuum with circular polarization can be generated from the oriented CO molecule. This enables the production sub-100 attosecond isolated pulse with the ellipticity as high as 0.9 at the macroscopic level. Moreover, the helicity of the generated high-order harmonics and the attosecond pulse can be tuned by adjusting the orientation of the CO molecule. This method will be beneficial for the studies on chiral-specific dynamics and magnetic circular dichroism on an attosecond time scale.     

Second harmonic stimulated Raman scattering of laser radiation in aplasma

A high-power linearly polarized laser propagating through a plasma produces oscillatory electron velocity at the second harmonic due to-the ν&oarr;×B&oarr; force, This velocity couples a Langmuir wave (ω, k&oarr;) and an electromagnetic wave (ω₁, k&oarr;₁), where ω₁=ω-2ω₀ , k-2k&oarr;₀ and ω₀, k&oarr;₀ are frequency and wavenumber of the laser pump, causing second harmonic Raman scattering. The growth rate is maximum for side scattering. This process can occur above the quarter critical density, unlike the first harmonic stimulated Raman scattering which occurs below the quarter critical density     

Orientation of polar molecules by laser induced adiabatic passage

We show that two overlapping linearly polarized laser pulses of frequencies omega and its second harmonic 2omega can strongly orient linear polar molecules, by adiabatic passage along dressed states. The resulting robust orientation can be interpreted as a laser-induced localization in the effective double well potential created by the fields, which induces a preliminary molecular alignment. The direction of the orientation can be selected by the relative phase of the fields.     

Broadband-Isolated Attosecond Pulse Generation by Two-Color Elliptically Polarized Laser Pulses

We numerically solve the two-dimensional Schrödinger equation and investigate isolated attosecond pulse generation by combining a left and a right elliptically polarized pulse together. It is found that the plateau of the harmonic spectra can be extended and the quantum paths can be controlled by adjusting ellipticity. A broadband width of about 220 eV is generated for the case that ellipticity equals 0.3, and time-frequency time–frequency analysis shows that only one long quantum path contributes to high-order harmonic generation. By superposing a bandwidth of 60 eV near the cutoff of the harmonic plateau, an attosecond pulse with the duration of about 62 as could be generated.     

Manipulating Nonlinear Photocurrent from Interlayer Coupling in Bilayer Metamaterials for Polarized Terahertz Generation

Polarized terahertz (THz) wave generation is of great significance for chiral and anisotropic sensing applications. However, how to manipulate amplitude, polarization, and ellipticity of the THz generation is still a fundamental challenge. Herein, polarized THz wave generation is achieved from a bilayer metamaterial consisting of T-shaped structure (TSS) and split resonator rings (SRRs) by combining Maxwell and hydrodynamic equations. The elliptically polarized THz wave can be synthetized directly from horizontally and vertically polarized THz components due to the orthogonal nonlinear photocurrents along the arm-directions of TSS and SRRs, respectively. Besides, the ellipticity and the orientation angle of the THz polarization ellipse can be modulated by the twist angle between the SRRs and TSS layers. The maximum ellipticity can reach 0.34 while the orientation angle is tunable from −0.45 to 0.48π by tuning the twist angle. This work proposes an interlayer coupling method for the polarized THz sources based on metamaterials in potential circular dichroism and chiral sensing applications.