高能量分辨光电子干涉仪研究进展

王慧勇; 李铭轩; 罗嗣佐; 丁大军

doi:10.7498/aps.74.20250534

摘要

近年来, 阿秒极紫外脉冲的产生与相关谱学测量技术的发展, 为研究电子动力学提供了强有力的工具. 阿秒时间尺度上的研究, 能够实时追踪原子分子的电子运动, 测量电子波包演变及其量子特性, 对于揭示电子在原子或分子内部的复杂动力学过程至关重要. 基于阿秒极紫外脉冲串光源发展起来的高能量分辨光电子干涉仪, 以其独特的高能量和高时间分辨特性在阿秒脉冲串光源的表征、原子分子光电离时间延迟、光电子量子态测量以及激光诱导电子动态干涉等动力学研究中实现了重要的应用. 本文围绕建立的先进阿秒串光源和高能量分辨电子谱学测量方法, 对高能量分辨的阿秒超快光电子干涉技术及其应用进行详细介绍, 并基于相关研究进展对阿秒光电子超快动力学以及量子系统相干调控的前景进行了展望.

关键词:

Abstract

In recent years, the attosecond extreme ultraviolet (XUV) pulse generation and advanced spectroscopic techniques have provided powerful tools for investigating electron dynamics. Researches on an attosecond timescale can realize real-time tracking of electronic motion in atoms and molecules, enabling the measurement of electron wave packet evolution and quantum characteristics, which are crucial for revealing complex dynamical processes within atomic and molecular systems. High-resolution photoelectron interferometers based on attosecond XUV pulse trains have played an important role in a wide range of applications due to their unique combination of high energy and temporal resolution. These applications include the characterization of attosecond pulse trains, the measurement of photoionization time delays in atoms and molecules, quantum state reconstruction of photoelectrons, and laser-induced electronic interference phenomena. By integrating attosecond temporal resolution with millielectronvolt level energy resolution, high-resolution photoelectron interferometric spectroscopy has emerged as a key technique for probing ultrafast dynamics and quantum state characterization. This review systematically summarizes recent advances in high-resolution attosecond photoelectron interferometry, with a focus on the experimental approaches and spectroscopic techniques required to access electron dynamics on an attosecond scale. These include the generation of narrowband attosecond XUV pulse trains, attosecond-stable Mach-Zehnder interferometers, high-energy resolution time-of-flight electron spectrometers, and quantum interference-based measurement schemes such as RABBIT and KRAKEN. This review discusses in detail the reconstruction of attosecond pulse sequences, shell-resolved photoionization time delay measurements in atoms, spectral phase evolution in Fano resonances, tomographic reconstruction of photoelectron density matrices on an attosecond timescale, and control experiments of laser-induced electronic dynamic interference effects. Through the analysis of recent studies, we demonstrate the powerful potential of attosecond high-energy resolution photoelectron interferometry in tracking ultrafast electron dynamics. Finally, the prospects of attosecond photoelectron spectroscopy in ultrafast dynamics and coherent manipulation of quantum systems are discussed.

Keywords:

作者及机构信息

吉林大学原子与分子物理研究所, 长春　130012

通信作者: 罗嗣佐, luosz@jlu.edu.cn ; 丁大军, dajund@jlu.edu.cn

基金项目: 国家重大科研仪器研制计划(批准号: 11627807)和国家自然科学基金(批准号: 12450402, 12134005)资助的课题.

Authors and contacts

Institute of Atomic and Molecular Physics, Jilin University, Changchun 130012, China

Corresponding author: LUO Sizuo, luosz@jlu.edu.cn ; DING Dajun, dajund@jlu.edu.cn

Funds: Project supported by the National Key Scientific Instrument and Equipment Development Project of China (Grant No. 11627807) and the National Natural Science Foundation of China (Grant Nos. 12450402, 12134005).

文章全文

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施引文献

图 1 (a) Ar与IR相互作用产生的窄带谐波光源; (b)窄带谐波H25的放大图; (c)阿秒极紫外脉冲串的时间结构示意图

Fig. 1. (a) Narrowband high-order harmonics generated by the interaction between Ar and the IR driving field; (b) magnified spectrum of the narrowband 25th harmonic (H25); (c) schematic illustration of the temporal structure of the attosecond extreme ultraviolet pulse train.

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图 2 (a)联合腔体内部光学元件与光束路径; (b)主动稳定系统下泵浦-探测臂延迟的绝对相位(上)与相对相位(下)测量结果. 黑色曲线表示在启用主动稳定系统时的长时间光束稳定性, 红色曲线则表示未启用主动稳定系统的情况^[40]

Fig. 2. (a) Optomechanical and beam path in the combination chamber; (b) absolute phase (upper) and relative phase (lower) of a pump-probe delay with active stability measurement. Long-term stability with (black) and without (red) feedback^[40].

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图 3 双光子跃迁量子路径干涉示意图, 使用了He原子的RABBIT光电子谱. 由XUV泵浦光激发的光电子在IR探测光的作用下额外吸收或辐射一个IR光子, 使主峰(MBs)的光电子跃迁至边带(SBs), 且光电子谱强度随XUV泵浦与IR探测之间的相对延迟发生振荡

Fig. 3. Schematic of two-photon transition quantum path interference, utilizing the RABBIT photoelectron spectrum of He atoms. The photoelectrons excited by the XUV pump laser, under the influence of the IR probe laser, absorb or emit an additional IR photon, shifting the photoelectrons from the main bands (MBs) to the sidebands (SBs). Furthermore, the intensity of the photoelectron spectrum oscillates as a function of the delay between the XUV pump and IR probe.

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图 4 (a) He原子的RABBIT光电子谱; (b) SB24的振荡数据信号与余弦拟合曲线; (c)提取不同SBs之间的相对相位; (d)基于ePIE算法对APTs进行重建, 得到脉冲持续时间约为280 as^[40]

Fig. 4. (a) RABBIT spectra of the He atom; (b) oscillatory signal of SB24 fitted with a cosine function; (c) extraction of relative phases between different sidebands; (d) reconstruction of APTs based on the ePIE, the pulse duration approximately 280 as^[40].

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图 5 (a) Ne原子中2s与2p壳层的光电离时间延迟差随光子能量的变化(黄点和红点), 与多体微扰理论计算(黑色实线)符合良好. 同时给出了阿秒条纹实验^[61]的结果(方块)和shake-up过程相对于2p光电离的时间延迟差(菱形). (b)实验所用光子谱图, 虚线为对应的透射曲线^[44]

Fig. 5. (a) Relative photoionization time delay between the 2s and 2p shells of Ne as a function of photon energy (yellow and red dots), exhibiting good agreement with the results of many-body perturbation theory (black solid line). The result from the attosecond streaking experiment^[61] (squares) is included, and the relative time delay between the shake-up process and 2p channel is shown in diamonds. (b) The photon spectrum used in the experiment, with the dashed line representing the corresponding transmission curve^[44].

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图 6 (a)实验测量中涉及的能级、通道和跃迁过程的示意图. 紫色(红色)箭头代表谐波(红外)光子, 黑色箭头代表自电离; 虚线代表吸收谐波光子或在吸收谐波光子后额外吸收或辐射红外光子到达连续态或虚态, 实线表示可能通过自电离衰变到准束缚态. 在Ar中的(b) SB18和(c) SB16中测量到的光电子能谱与XUV和IR之间延迟的函数关系. (d) SB18和(e) SB16中的光电子能谱减去振荡平均值^[53]

Fig. 6. (a) Illustration of the levels, channels, and transition processes involved in the experiment. The purple (red) arrows represent the harmonic (IR) photons. The black arrows indicate autoionization. Dashed lines mark continuum or virtual states reached by absorption of a harmonic or a harmonic ± an IR photon. Solid lines are quasibound states which may decay by autoionization. Measured photoelectron spectra in (b) SB18 and (c) SB16 in argon as a function of delay between XUV and IR. Photoelectron spectra in (d) SB18 and (e) SB16 after subtracting the mean values of the oscillations^[53].

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图 7 KRAKEN技术电离He原子的实验结果　(a)不同$ {\text{δ}}\omega $探测光梳的光电子能谱图; (b)不同$ \hbar {\text{δ}} \omega $光谱图的振荡振幅$ A_{{\text{δ}} \omega} $; (c)重构得到的密度矩阵^[30]

Fig. 7. Experimental results of ionizing He atoms using KRAKEN technique: (a) Photoelectron spectra with different ${\text{δ}} \omega $ probe frequency combs; (b) the oscillation amplitude $ A_{{\text{δ}} \omega} $ for the spectra corresponding to different $ \hbar {\text{δ}} \omega $ values; (c) reconstruction of the density matrix^[30].

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图 8 根据实验测量和理论计算对He的密度矩阵进行重构　(a)根据实验测量结果重构的密度矩阵; (b)检索光谱仪响应函数后, 根据实验结果重构的密度矩阵; (c)基于RRPAE计算重构的密度矩阵; (d)基于RRPAE计算下单光子电离重构得到的密度矩阵^[30]

Fig. 8. Reconstruction of the density matrix for He based on experimental measurements and theoretical calculations: (a) The density matrix reconstructed from experimental measurement results; (b) the density matrix reconstructed from experimental results after retrieving the corresponding function of the spectrometer; (c) the density matrix reconstructed based on RRPAE calculations; (d) the density matrix reconstructed based on single-photon ionization under RRPAE calculations^[30].

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图 9 (a) 实验、(b) TDSE和(c) SFA中获得的电离He原子产生的光电子能谱与泵浦探测时间延迟的关系^[31]

Fig. 9. Photoelectron spectra from ionization of He as a function of time delay between pump and probe lasers, which are obtained in (a) experiment, (b) TDSE, and (c) SFA, respectively^[31].

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