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飞行时间光电子谱仪(time-of-flight photoelectron spectrometer, TOF-PES)作为超快电子动力学研究的核心工具, 凭借其数十皮秒量级的飞行时间分辨率与宽能量探测范围, 在阿秒脉冲表征与强场量子过程研究中提供了不可替代的技术支撑. 本文尝试系统地总结飞行时间光电子谱仪的技术原理与发展历程, 探讨磁瓶式高分辨率谱仪技术在电子轨迹控制与收集效率提升方面的突破, 并结合双光子跃迁干涉阿秒拍频重构、阿秒条纹相机等实验技术分析其在阿秒脉冲表征中的关键作用. 此外, 还介绍了TOF技术与其他高精度探测手段之间的融合应用, 包括角分辨光电子能谱、冷靶反冲离子动量谱仪及速度成像谱仪, 展示其在获取多维电子动力学信息方面的潜力. 最后对TOF技术瓶颈以及未来发展方向进行了探讨.
Time-of-flight photoelectron spectroscopy (TOF-PES) with exceptional energy and temporal resolution has emerged as a cornerstone diagnostic tool in attosecond science and ultrafast dynamics. This work comprehensively reviews the TOF-PES technology, its basic principles, and its crucial role in attosecond metrology. The first part in this paper introduces the historical development of TOF methods, from early ion mass spectrometry to modern photoelectron applications, detailing key innovations such as energy and spatial focusing, magnetic shielding, and delay-line detectors. The implementation of magnetic bottle spectrometers (MBES) is discussed in depth, emphasizing their advantages in wide-angle electron collection and improving energy resolution through trajectory collimation and magnetic gradient design. We then focus on the application of TOF-PES in attosecond pulse characterization, particularly in the RABBITT(reconstruction of attosecond beating by interference of two-photon transitions, and attosecond streaking techniques. A broad array of experimental breakthroughs is reviewed, including ultrafast delay scanning, energy-time mapping through photoelectron modulation, and the use of MBES to analyze the phase and amplitude of attosecond pulse trains with accuracy below 50 attosecond. These advances indicate that the TOF-PES is a key driving factor for temporal phase reconstruction and group delay measurement in an extreme-ultraviolet (XUV) spectral range. Then the integration of TOF-based detection in time- and angle-resolved photoemission spectroscopy (TR-ARPES and ARTOF) is explored, making it possible to realize the full 3D momentum-resolved detection without mechanical rotation or slits. The synergistic effect between TOF and ultrafast laser sources promotes the simultaneous resolution of energy and momentum resolution in the Brillouin zone, with applications covering topological materials, superconductors, and charge-density wave systems. Finally, this review extends to momentum-resolved ultrafast electron-ion coincidence techniques. The use of TOF in COLTRIMS (cold target recoil ion momentum spectroscopy) and VMI (velocity map imaging) is evaluated, highlighting its indispensable role in resolving related electron-ion dynamics, few-body fragmentation processes, and tunneling time delays on attosecond and even zeptosecond scales. Overall, this work emphasizes the central role of TOF-PES in advancing the frontiers of ultrafast science. Although current challenges include space-charge effects, detector response limitations, and data handling complexity, future advances in quantum detection, AI-driven trajectory correction, and high-repetition-rate light sources are expected to overcome these barriers. TOF-PES, through its continuous evolution, is still a key platform for detecting quantum dynamics on the fastest known timescale. -
Keywords:
- time-of-flight photoelectron spectrometer /
- attosecond pulse characterization /
- angle-resolved photoelectron spectroscopy /
- ultrafast electron dynamics
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图 4 电子谱仪的比较 (a) 半球形分析仪; (b) 角分辨飞行时间谱仪
Fig. 4. Comparison of electron spectrometers: (a) Hemispherical analyzer; (b) angle-resolved time-of-flight spectrometer.
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