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在过去20年里, 激光技术的发展使阿秒科学成为一个新的研究领域, 可为量子少体超快演化过程的研究提供新视角. 当前实验室中制备的阿秒脉冲以孤立脉冲或脉冲串的形式被广泛应用于实验研究中, 其超快变化的光场允许人们操控和跟踪电子在原子尺度的运动, 实现对亚飞秒时间尺度电子动力学的实时追踪. 本综述聚焦于阿秒科学的重要组成部分, 即原子分子超快动力学研究的进展. 首先介绍阿秒脉冲的产生和发展, 主要包括高次谐波原理和孤立阿秒脉冲分离方法; 然后系统地介绍阿秒脉冲在原子分子超快动力学研究中的应用, 包括光电离时间延迟、阿秒电荷迁移和非绝热分子动力学等方面; 最后对阿秒脉冲在原子分子超快动力学研究中的应用进行总结和展望.In the past two decades, the development of laser technology has made attosecond science become a cutting-edge research field, providing various novel perspectives for the study of quantum few-body ultrafast evolution. At present, the attosecond pulses prepared in laboratories are widely used in experimental research in the form of isolated pulses or pulse trains. The ultrafast changing light field allows one to control and track the motions of electrons on an atomic scale, and realize the real-time tracking of electron dynamics on a sub-femtosecond time scale. This review focuses on the research progress of ultrafast dynamics of atoms and molecules, which is an important part of attosecond science. Firstly, the generation and development of attosecond pulses are reviewed, mainly including the principle of high-order harmonic and the separation method of single-attosecond pulses. Then the applications of attosecond pulses are systematically introduced, including photo-ionization time delay, attosecond charge migration, and non-adiabatic molecular dynamics. Finally, the summary and outlook of the application of attosecond pulses are presented.
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Keywords:
- high-order harmonic /
- attosecond science /
- pump-probe /
- ultrafast dynamics
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图 4 (a) ZnO晶体HHG谱, 其中绿色和蓝色曲线分别表示驱动脉冲能量为0.52 µJ和2.63 µJ产生的谐波谱, 插图为2.63 µJ谐波谱的截止点及其附近的展开图[62]; (b) 高能截止点与驱动激光电场的线性关系[62]; (c1)固相Ar的HHG谱, 展示了低强度(16 TW/cm2)下的单平台和较高强度(26 TW/cm2)下的双平台[75]; (c2)固相Kr的HHG谱, 谐波谱(11.4 TW/cm2)由不同谱仪分别获取的两个光谱连接而成[75]
Fig. 4. (a) HHG spectrum of ZnO crystal, the green and blue curves represent the HHG spectrum generated by the driving pulse energies of 0.52 µJ and 2.63 µJ, and the inset shows the expanded view at and near the cutoff of the 2.63 µJ spectrum[62]; (b) high-energy cutoff scales linearly with drive-laser electric field[62]; (c1) HHG spectra from solid Ar, and single-platform at low intensity (16 TW/cm2) and dual-platform at higher intensity (26 TW/cm2) are shown[75]; (c2) HHG spectra from solid Kr, and the spectrum (11.4 TW/cm2) is composed of two spectra taken by different spectrometers[75].
图 5 线偏振少周期激光产生的相干XUV和软X射线辐射 (a)最高能量光子在脉冲峰值附近出射, 蓝线(
$\varphi = 0$ )和红线($\varphi = {\text{π }}/2$ )分别为不同CEP下的脉冲发射[116]; (b)不同CEP下X射线光谱截止区的连续性(蓝线,$\varphi = 0$ )和准周期性(红线,$\varphi = {\text{π }}/2$ )特征[116]; (c)振幅选通示意图[8]Fig. 5. Coherent XUV and soft-X-ray radiation generated by a linearly polarized, few-cycle light pulse: (a) Highest-energy photons are emitted near the pulse peak, the blue line (
$\varphi = 0$ ) and the red line ($\varphi = {\text{π }}/2$ ) are the pulse emission under different CEPs, respectively[116]; (b) the continuous (blue line,$\varphi = 0$ ) and quasi-periodic (red line,$\varphi = {\text{π }}/2$ ) features of the X-ray spectral distribution in the ‘cut-off ’ range under different CEPs[116]; (c) schematic of amplitude gating[8].
图 6 HCOs [124]和电离选通的原理示意图[126] (a)左侧: 由SFA计算得到的两周期激光脉冲电场(虚线)与对应的HCO电子轨迹. 灰度表示发射轨迹的相对强度. 右侧: 利用量子轨道模型分离出单个轨迹对应的谐波谱和截止位置. (b)在不同激光脉冲强度(虚线)下计算得到的相位匹配因子 (蓝线). 灰线表示介质的对应电离程度. 蓝色方格为从HCO中提取的脉冲强度. 左右图框分别对应7 fs, 6.7×1014 W/cm2和10 fs, 1.1×1015 W/cm2高斯脉冲拟合的强度包络
Fig. 6. Schematic diagram of the HCOs[124] and the ionization gating[126]. (a) Left: the electric field of a two-cycle laser pulse (dashed line) with the corresponding HCO electron trajectories, calculated by the SFA. The grey scale indicates the relative intensity of emission trajectories. Right: using the quantum orbital model to isolate the harmonic spectrum and cut-off position corresponding to a single trajectory. (b) Calculated phase matching factor (blue line) at different laser pulse intensities (dashed line). The corresponding ionization of extent of the medium is represented by gray lines. Blue squares are pulse intensities extracted from the HCOs. The left and right frames correspond to the intensity envelopes fitted by the 7 fs, 6.7×1014 W/cm2 and 10 fs, 1.1×1015 W/cm2 Gaussian pulses, respectively.
图 7 时间选通示意图[98] (a)偏振选通(上)和双光选通(下); (b)多周期驱动光场(蓝线)产生的APT, 单色驱动下的半个光周期脉冲间隔(上)和双色驱动下的完整光周期脉冲间隔(下)
Fig. 7. Schematic diagram of the temporal gating[98]: (a) Polarization gating (top) and double optical gating (bottom); (b) APT is generated by a multi-cycle driving field (blue curves), the half photo-period pulse intervals under monochromatic drive (top) and the complete photo-period pulse intervals under two-color drive (bottom).
图 8 (a)广义双光选通装置[151] (光学器件由石英片(QP1)、一个布儒斯特窗(BW)、第二个石英片(QP2)和一个BBO晶体组成); (b)双迈克耳孙干涉仪[155] (BS, 分束器; M, 平面反射镜; TS1—3, 压电平移台; A, 光强衰减器; First M1和Second M2, 第一台和第二台迈克尔逊干涉仪)
Fig. 8. (a) Generalized double optical gating[151] (The optics consist of a quartz plate (QP1), a Brewster window (BW), a second quartz plate (QP2), and a BBO crystal); (b) dual Michelson interferometer[155] (BS, beam splitters; M, flat mirrors; TS1—3, piezoelectric translation stages; A, intensity attenuator; First M1 and second M2, the first and the second Michelson interferometers).
图 9 阿秒灯塔示意图 (a) 等离子体镜中谐波产生的阿秒灯塔效应[160] (a1) 阿秒脉冲沿垂直于焦点处激光波前的方向传播(左); WFR导致阿秒脉冲发生空间分离(右); (a2) WFR效应示意图; (a3) 等离子体镜阿秒灯塔实验示意图. (b) 气体靶阿秒灯塔实验示意图[161], 角色散在聚焦前被一对错位楔形施加在激光束上在焦点产生空间啁啾, 激光脉冲每个半周期内产生的阿秒脉冲沿不同方向传播
Fig. 9. Schematic diagram of attosecond lighthouses. (a) Attosecond lighthouse effect in harmonics generated from a plasma mirror[160]: (a1) The attosecond pulse propagates in a collimated beam perpendicular to the laser wavefront at the focal point (left); WFR leads to spatial separation of attosecond pulses (right); (a2) schematic diagram of the WFR effect; (a3) schematic diagram of the plasma mirror attosecond lighthouse experiment. (b) Schematic diagram of the gas target attosecond lighthouse experiment[161]. Angular dispersion is imposed on the laser beam before focusing using a misaligned pair of wedges, leading to spatial chirp at the focus. The attosecond pulses generated in each half-cycle of the laser pulse propagate in different directions.
图 10 (a) 780 nm, 8 fs驱动脉冲在Ar气中产生的HHS[173], 三个面板对应的激光强度分别为 ① 2.5×1014 W/cm2, ② 2.9×1014 W/cm2, ③ 3.5×1014 W/cm2. (b) Xe的多电子动力学示意图[176], 电子以两种不同的方式与离子重新结合 (b1) 电子与5p壳层的空穴结合; (b2) 电子与4d壳层的空穴结合. (c) N2, O2和CO2的HHS[186], 其中100 fs, 800 nm的激光脉冲实现气相分子定向, 另一束更强的800 nm激光脉冲电离分子产生HHS. 横轴表示高次谐波脉冲的偏振平行于分子轴, 半径范围为0—50的谐波阶次
Fig. 10. (a) HHS generated in argon using an 8 fs laser pulse centered at 780 nm[173]. The three different panels correspond to the laser intensities 2.5×1014 W/cm2 ①, 2.9×1014 W/cm2 ②, 3.5×1014 W/cm2 ③. (b) Schematic diagram of multi-electron dynamics in xenon[176]. The electron recombines with the ion in two different ways: the electron recombines with the hole in 5p shell (b1) and in 4d shell (b2). (c) HHS of molecules N2, O2 and CO2[186]. The gas-phase molecules are aligned by a 100 fs, 800 nm laser pulse, and ionized by another stronger 800 nm laser pulse to generate HHS. The horizontal axis denotes that the high-harmonic pulse’s polarization axis is parallel to the molecular axis, and the radius covers harmonic orders from 0 to 50.
图 11 分子轨道层析成像 (a) N2分子的HOMO的图像[183], 分子轴沿水平方向 (a1)使用层析重建算法从一系列角度下实验HHS中得到的轨道波函数图像; (a2) 使用量子化学包计算的
$3{\sigma _{\text{g}}}$ 轨道波函数图像. (b) N2最高的两个分子轨道的重建图像[192](b1) 利用复合偶极子的虚部并施加${\sigma _{\text{g}}}$ 对称性还原的HOMO; (b2)利用复合偶极子的实部并施加πu对称性还原的HOMO-1; (b3), (b4) 分别是用GAMESS 计算的Hartree-Fock HOMO和HOMO-1. (c) CO2中HOMO的轨道重建[193], 分子轴沿垂直方向 (c1) 根据广义层析方法从实验数据中检索的HOMO图像; (c2) 用量子化学程序计算出的CO2中HOMO的二维投影Fig. 11. Tomographic imaging of molecular orbitals. (a) Image of HOMO of a N2 molecule[183], the molecular axis is horizontal: (a1) Shows the orbital wavefunction image derived from the experimental HHS at a range of angles using the tomographic reconstruction algorithm; (a2) shows the
$3{\sigma _{\text{g}}}$ orbital wavefunction image calculated with a quantum chemistry package. (b) Reconstructed images of the highest two molecular orbitals of N2[192]: (b1) HOMO is recovered by using the imaginary part of the recombination dipole and imposing${\sigma _{\text{g}}}$ -symmetry; (b2) HOMO-1 is recovered by using the real part of the recombination dipole and imposing πu-symmetry; (b3), (b4) Hartree-Fock HOMO and HOMO-1 calculated with GAMESS, respectively. (c) HOMO reconstruction of CO2[193], the molecular axis is vertical: (c1) HOMO image retrieved from the experimental data following the generalized tomographic procedure; (c2) bidimensional projection of the HOMO of CO2 calculated with a quantum chemistry program.
图 12 Pump-probe方案[208] (紫色区域表示阿秒XUV脉冲包络, 红色区域表示一个probe激光脉冲, 红色虚线是probe脉冲对应的电场) (a) 传统pump-probe方案, 从不同延迟probe脉冲下的重复实验[209,210]中实时提取出关于系统无场传播的时间信息; (b) SAP和少周期IR场的pump-probe实验; (c) APT和单色IR场的pump-probe实验
Fig. 12. Pump-probe schemes[208] (The purple area represents the attosecond XUV pulse envelope and the red area represents the one of the probing laser pulses, while the dotted red lines indicate the corresponding E-field): (a) Traditional pump-probe experiment, the temporal information about the field-free propagation of the system, can then be extracted in real time by repeating the experiment systematically for different delays of the probe pulse[209,210]; (b) simultaneous pump-probe experiment between a SAP and a few-cycle IR field; (c) simultaneous pump-probe experiment between an APT and a monochromatic IR field.
图 13 (a) 提取光电离时间延迟的阿秒条纹的典型图像[3] (a1) 阿秒脉冲(蓝线)和条纹IR脉冲的矢势(红线); (a2) 平行于激光偏振的电子动量分布
${p_z}$ 随两个脉冲之间时间延迟$\tau $ 的变化(中央的白色曲线代表瞬时动量分布${\bar p_z}$ , 插图展示了${\bar p_z}$ 和IR矢势间峰值的差异, 其为条纹时间延迟${\tau _{\text{S}}}$ ). (b) He原子的阿秒条纹实验[227], 左侧表示结合能为24.6 eV的He原子基态; 中间表示He+ 1s1(shake-down)态离子势, 由于一个电子被电离, 剩余的电子会重新分布并占据更紧密的束缚态; 右侧表示He+2s1/2p1(shake-up)态离子势, 一个电子出射, 剩余电子被激发到一系列shake-up态n (插图表示He原子单电离阿秒条纹图像)Fig. 13. (a) Typical configurations of the attosecond streaking for extraction of the photoionization time delay[3]: (a1) The vector potential of the attosecond pulse (blue line) and the streaking IR pulse (red line); (a2) electron momentum distribution parallel to the laser polarization
${p_z}$ as a function of the time delay$\tau $ between the two pulses, where the central white curve stands for the first moment of the momentum distribution${\bar p_z}$ . The insert shows the difference between the peaks of the${\bar p_z}$ and the IR vector potential is the streaking time delay${\tau _{\text{S}}}$ . (b) Attosecond streaking spectroscopy of helium[227]: Left panel is the helium ground state with a binding energy of 24.6 eV; the middle panel represents the ion potential of the He+ 1s1 (shake-down) state (The ionic potential rearranges as result of an electron loss, and the remaining electron occupies a more tightly bound state); the right panel represents the ion potential of He+ 2s1/2p1 (shake-up) state, and the electron emission can be accompanied by the excitation of the remaining electron into one out of a series of shake-up states n (The inset shows the single ionization attosecond streaking image of helium).
图 14 (a), (b) Ar的 3s和3p壳层相对电离时间延迟的测量[215] (a) RABBIT原理示意图; (b1), (b2) 分别为3s壳层和3p壳层释放的电子能谱随脉冲时间延迟的变化; (b3) 修正Cr滤波器群延迟后的3p壳层延迟(虚线)与3s壳层延迟的对比. (c) Ar光电离时间延迟对电子出射角度的依赖和光电子角分布的延迟依赖的测量[229] (c1), (c2) 分别为实验和理论中不对称参数
${\beta _2}$ 随延迟的变化; (c3)实验(圆圈)和理论(实线)中原子延迟的角依赖关系 (不同的边带表示为14ω(蓝色), 20ω(品红色)和22ω(黄色))Fig. 14. (a), (b) Measurement of relative ionization time delay of 3s and 3p shells of Ar[215]: (a) Schematic diagram of RABBIT principle; (b1), (b2) energy spectra as a function of pulse time delay from electrons liberated from the 3s shell and the 3p shell, respectively; (b3) after correcting the Cr filter group delay, comparison of the 3p shell delay (dashed line) versus the 3s shell delay. (c) The electron emission angular dependence of the photoionization time delay and the delay dependence of the photo-electron angular distribution are measured in Ar[229]: (c1), (c2) Experimental and theoretical variation of the asymmetric parameters
${\beta _2}$ as a function of delay; (c3) experimental (circles) and theoretical (solid curves) angle dependence of the atomic delay (Different sidebands are indicated as 14ω (blue), 20ω (magenta) and 22ω (yellow)).
图 15 (a1), (a2)分别表示H2在XUV-IR作用下不对称电离解离的两种机制[233], 蓝色和红色箭头分别表示EUV脉冲和IR脉冲的影响, 紫色线和箭头表示分子固有动力学. (b)氨基酸中发生的纯电子动力学行为[15] ①二价亚胺离子的产量随pump-probe延迟的变化; ②位于①中虚线框所示的时间窗口内; ③表示实验数据同①中指数拟合曲线的差值, 红色曲线为频率为0.234 PHz的正弦函数. (c) 准无场CM的重建[237] ①重建的HCCI分子电离后随时间变化的电子动力学过程; ②, ③分别为在分子垂直排列和平行排列下, 电离时空穴密度的重建
Fig. 15. (a1), (a2) Represent the two mechanisms of asymmetric ionization dissociation of H2 under the action of XUV-IR, respectively[233]. Blue and red arrows indicate the effects of EUV and IR pulses respectively. Purple lines and arrows signify dynamics that is intrinsic to the molecule. (b) Pure electron dynamics occurring in amino acids[15]: ① Yield of doubly charged immonium ion as a function of pump-probe delay[15]; ② within the temporal window shown as dotted box in ①; ③ difference between the experimental data and the exponential fitting curve displayed in ①, red curve is a sinusoidal function of frequency 0.234 PHz. (c) Reconstruction of quasi-field-free CM[237]: ① The reconstructed electron dynamics of HCCI molecule are displayed as a function of time after ionization; ②, ③ the reconstructed hole density at the time of ionization is shown for perpendicular and parallel alignment, respectively.
图 16 (a) HHG瞬态光栅光谱实验装置[249] (a1) 瞬态光栅实现激发态与非激发态分子布居的空间调制导致谐波在远场产生一阶衍射图像; (a2) 探测分子锥形交叉动力学中电子特性的原理, 激发态(蓝色波包)分子有强的衍射图样, 布居转移产生的基态(红色波包)分子衍射强度减弱. 上图为瞬态光栅的空间强度结构, 下图表示NO2最低的两个势能面. (b1) CH3Br的中性激发态动力学ATAS 图像[258]; (b2) CH3Br中性激发态的ATAS动力学模拟[258]; (b3) CH3Br的基态、激发态和Rydberg态势能曲线, 粗体彩色曲线表示构成激发带的主要能态, 在
$^1{Q_1}$ 和$^{\text{3}}{Q_{\text{0}}}$ 激发态间存在的CIs导致产物为Br和Br*的两个解离路径之间的布局转移[258]. (c) C4H${}_3^+ $ 碎片产额随XUV-VIS/NIR延迟(红点)的变化[255], 黑线是对实验数据的双指数拟合, 虚线表示两个时间尺度的贡献; 插图显示了C4H${}_3^+ $ 的大范围pump-probe扫描Fig. 16. (a) Experimental setup for HHG transient grating spectroscopy[249]: (a1) A first-order diffraction image of harmonics in the far field, caused by the spatial modulation of excited and unexcited molecularpopulations realized by transient gratings; (a2) principles for probing the electronic character of the molecule during the conical intersection dynamics, molecules in the excited state (indicated by blue wave packets) have a strong diffraction pattern, and the diffraction intensity of the ground state (indicated by red wave packets) generated by population transfer is decreased. The top illustrates the spatial intensity structure of the transient grating, and the bottom shows schematically the lowest two potential energy surfaces of NO2. (b1) ATAS image of the neutral excited state dynamics in CH3Br[258]; (b2) simulated ATAS dynamics for neutral excited states in CH3Br[258]; (b3) different potential energy curves for CH3Br, the bold color curves represent the primary states that compose the excited state band, CIs exist between the
$^1{Q_1}$ and$^{\text{3}}{Q_{\text{0}}}$ excited states that can lead to population transfer between the two dissociation paths with products Br and Br*[258]. (c) C4H${}_3^+ $ fragment yield as a function of the XUV-VIS/NIR delay (red dots)[255], the bold black line is a biexponential fit to the data, and the dashed lines represent the contributions from the two timescales. The inset displays a long range pump-probe scan of C4H${}_3^+ $ . -
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