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.     

Electron localization of H_2~+ in a dc electric field

A dc electric field is utilized to steer the electron motion after the molecular ion H_2~+ is excited by an ultrashort ultraviolet laser pulse. The numerical simulation shows that the electron localization distribution and the dissociation control ratio are dependent on the polarization direction and amplitude of the dc electric field. Most electrons of the dissociation state move opposite to the dc electric field and stabilize at the dressed-up potential well, for the dressed-down well is occupied by the electrons of the 1 sσ_g state.     

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.     

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.     

影响单电子非线性汤姆孙散射因素的研究

应用电子汤姆孙散射的经典理论，通过理论分析和计算机模拟，研究了超短超强激光脉冲作用下电子产生的辐射脉冲的性质.计算表明，在这种情况下，电子的辐射通常以阿秒脉冲列的形式出现.讨论了不同激光场参数（包括激光强度、脉宽、初相位和偏振态）、不同电子初始状态（初始速度和位置）对辐射脉冲的时间和空间特性的影响.通常在相对论光强条件下，激光强度越大，电子辐射越强，脉宽越窄，中心频率越大，并且方向性越好；电子在线偏振激光中产生的辐射效率，比在同样强度下圆偏振激光中产生的效率更高；无论入射光是线偏振光，还是圆偏振光,辐射场呈现较复杂的偏振态, 并且它与辐射方向有关.当电子具有一定的初始能量时，通常辐射场的振幅随电子初始能量的增大而增大.不管电子的初始能量以及运动方向如何，做相对论运动的电子产生的辐射趋向于出现在靠近电子运动方向的角度区域.     

Polarization state of high-order harmonic emission from aligned molecules

High harmonic emission in isotropic gases is polarized in the same direction as the incident laser polarization. Laser-induced molecular alignment allows us to break the symmetry of the gas medium. By using aligned molecules in high harmonic generation experiments, we show that the polarization of the extreme ultraviolet emission depends strongly on the molecular alignment and the orbital structure. Polarization measurements give insight into the molecular orbital symmetry. Furthermore, molecular alignment will allow us to produce attosecond pulses with time-dependent polarization.     

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.     

NH4H2PO4和ND4D2PO4晶体微结构的拉曼光谱研究

本文利用偏振拉曼光谱和第一性原理, 对磷酸二氢铵(NH₄H₂PO₄, ADP)和不同氘含量磷酸二氢铵DADP晶体的晶格振动模式进行了研究. 实验测得了不同几何配置、200–4000 cm^-1范围的偏振拉曼光谱, 分析在不同氘含量条件下921 cm^-1和3000 cm^-1附近拉曼峰的变化. 在ADP晶体中, 基于基本结构单元NH₄⁺ 和H₂PO₄^-基团的振动模, 用第一性原理进行了数值模拟, 进一步明确拉曼峰与晶体中原子振动的对应关系; 通过洛伦兹拟合不同氘含量DADP晶体的拉曼光谱中2000–2600 cm^-1处各峰的变化讨论了DADP 晶体的氘化过程, 结果表明氘化顺序是先NH₄⁺ 基团后H₂PO₄^-基团, 研究结果为今后此类材料的生长和性能优化奠定了基础.     

Probing the spatial structure of a molecular attosecond electron wave packet using shaped recollision trajectories

Using orthogonally polarized 800 nm and 400 nm laser pulses, we have generated high harmonics in ethane (C(2)H(6)). We observe that the intensity of each harmonic order modulates with the attosecond delay between the two laser fields. The modulation period of the low even harmonics is twice that of the period of modulation of the other harmonics. By comparing with theoretical calculation, we show that the double periodicity is a result of the electron wave packet motion in the valence shell of C(2)H(6) on the attosecond time-scale. Our method is a general approach to measuring internal electron dynamics which does not require molecular alignment, making it applicable to more complex molecules than previous approaches.     

N_2-H_2容性耦合等离子体电非对称效应的particle-in-cell/Monte Carlo模拟

H_2-N_2混合气体电容性耦合射频放电在有机低介电系数材料刻蚀中具潜在研究意义.采用paxticle-incell/Monte Carlo模型模拟了双频(13.56 MHz/27.12 MHz)电压源分别接在结构对称的两个电极上的H_2-N_2容性耦合等离子体特征,研究了其电非对称效应.模拟结果表明,通过调节两谐波间的相位角θ,可以改变其电场、等离子体密度、离子流密度的轴向分布及离子轰击电极的能量分布.当相位角θ为0°时,低频电极(晶片)附近主要离子(H_3~+)的密度最小,离子(H_3~+,H_2~+,H~+)轰击低频电极的流密度及平均能量最高;当θ从0°变化90°时,低频电极的自偏压从-103V到106V近似线性增加,轰击电极的离子流密度变化约±18%,H~+离子轰击低频电极的最大能量约减小2.5倍,轰击电极的平均能量约变化2倍,表明氢离子能量和离子流几乎能独立控制.     

Electron localization of linear symmetric molecular ion H_3~(2+)

Electron localization in the dissociation of the symmetric linear molecular ion H_3~(2+) is investigated. The numerical simulation shows that the electron localization distribution is dependent on the central frequency and peak electric field amplitude of the external ultrashort ultraviolet laser pulse. When the electrons of the ground state are excited onto the 2pσ~2Σ_u~+ by a one-photon process, most electrons of the dissociation states are localized at the protons on both sides symmetrically. Almost no electron is stabilized at the middle proton due to the odd symmetry of the wave function. With the increase of the frequency of the external ultraviolet laser pulse, the electron localization ratio of the middle proton increases, for more electrons of the ground state are excited onto the higher 3pσ~2Σ_u~+ ustate. 50.9% electrons of all the dissociation events can be captured by the middle Coulomb potential well through optimizing the central frequency and peak electric field amplitude of the ultraviolet laser pulse. Besides, a direct current(DC) electric field can be utilized to control the electron motions of the dissociation states after the excitation of an ultraviolet laser pulse, and 68.8% electrons of the dissociation states can be controlled into the middle proton.     

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.     

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.     

不同偏振态下的飞秒激光脉冲与铝靶相互作用中超热电子的产生

研究了P偏振、S偏振和圆(C)偏振态下亚相对论强度飞秒激光脉冲与铝靶相互作用时产生的超热电子的能谱和靶背向角分布，并对S偏振产生的超热电子的特殊角分布通过引入表面磁场的概念进行了定性解释. 关键词： 超短超强激光 等离子体 超热电子 表面磁场     

Harmonic spectra bandwidth broadening with a new polarization gating

A new polarization gating is demonstrated by our principle-of-proof experiment, which is theoretically proposed to generate the isolated or double attosecond pulses with the multi-cycle driving laser pulse in the previous work [Optics Express. 20, 5196 （2012）]. In the experiment, the polarization gating is formed by two orthogonally-polarized linearly chirped multi-cycle laser pulses, and the spectral bandwidths of tile harmonics are broadened by more than two times, which agree with the previous theoretical work.     

大气压甲烷针-板放电等离子体中粒子密度和反应路径的数值模拟

甲烷针-板放电与重油加氢耦合形成甲烷转化重油加氢,可实现重油高效加氢并增产高附加值低碳烯烃,有实践应用前景和科学研究意义.建立二维流体模型,对大气压甲烷针-板放电等离子体进行数值模拟,得到电场强度、电子温度和粒子密度的空间与轴向分布,总结反应产额并提炼生成各种带电和中性粒子的关键路径.模拟结果表明,CH_3~+和CH_4~+密度与电场强度和电子温度的轴向演化接近且密切相关;CH_5~+和C_2H_5~+密度沿轴向先增大后减小;CH_3与H密度的空间和轴向分布几乎相同;CH_2,C_2H_4与C_2H_5的粒子密度分布在靠近阴极的区域内明显不同而在正柱区内较为相像;电子与CH_4发生电子碰撞电离生成的CH_3~+和CH_4~+,CH_3~+和CH_4~+分别与CH_4发生分子碰撞解离生成C_2H_5~+和CH_5~+;电子与CH_4间的电子碰撞分解是生成CH_3,CH_2,CH和H的主导反应;CH_2与CH_4和电子与C_2H_4发生的反应分别是生成C_2H_4和C_2H_2的关键路径;电子与CH_4间的电子碰撞分解反应和CH_2与CH_4发生的反应的产额各占H_2总产额的52.15%和47.85%.     

飞秒激光在6H SiC晶体表面制备纳米微结构

激光诱导周期性纳米微结构在多种材料包括电介质、半导体、金属和聚合物中观察到。研究了800nm和400nm飞秒激光垂直聚焦于6H SiC晶体表面制备纳米微结构。实验观察到800nm和400nm线偏光照射样品表面分别得到周期为150nm和80nm的干涉条纹,800nm圆偏振激光单独照射样品表面得到粒径约100nm的纳米颗粒。偏振相互垂直的800nm和400nm激光同时照射晶体得到粒径约100nm的纳米颗粒阵列,该纳米阵列的方向随400nm激光强度增加而向400nm偏振方向偏转。利用二次谐波的观点对以上纳米结构的形成给出了解释。     

Controlling high harmonic generation with molecular wave packets

We show that, by controlling the alignment of molecules, we can influence the high harmonic generation process. We observed strong intensity modulation and spectral shaping of high harmonics produced with a rotational wave packet in a low-density gas of N2 or O2. In N2, where the highest occupied molecular orbital (HOMO) has sigma(g) symmetry, the maximum signal occurs when the molecules are aligned along the laser polarization while the minimum occurs when it is perpendicular. In O2, where the HOMO has pi(g) symmetry, the harmonics are enhanced when the molecules are aligned around 45 degrees to the laser polarization. The symmetry of the molecular orbital can be read by harmonics. Molecular wave packets offer a means of shaping attosecond pulses.     

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.     

基于半解析自洽理论研究相对论激光脉冲驱动下阿秒X射线源的产生

发展了一种描述相对论激光脉冲与稠密等离子体相互作用产生阿秒X射线源的半解析自洽理论.该理论模型不仅可以获得等离子体界面的振荡轨迹、振荡面电场和磁场等物理参数,而且能够精确计算出激光脉冲驱动下阿秒X射线源的频谱,结果与粒子模拟程序一致.理论计算结果表明阿秒X射线源的辐射特性与等离子体界面随时演化过程相关,在周期量级激光场驱动下等离子体界面振荡振幅呈现中心不对称,通过改变激光场的载波包络相位实现对等离子体界面振荡的控制,获得准单阿秒X射线源.