Influence of Photoemission Geometry on Timing and Efficiency in 4D Ultrafast Electron Microscopy.

IF 2.3 3区 化学 Q3 CHEMISTRY, PHYSICAL Chemphyschem Pub Date : 2025-01-13 DOI:10.1002/cphc.202401032
Simon A Willis, David J Flannigan
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Abstract

Broader adoption of 4D ultrafast electron microscopy (UEM) for the study of chemical, materials, and quantum systems is being driven by development of new instruments as well as continuous improvement and characterization of existing technologies. Perhaps owing to the still-high barrier to entry, the full range of capabilities of laser-driven 4D UEM instruments has yet to be established, particularly when operated at extremely low beam currents (~fA). Accordingly, with an eye on beam stability, we have conducted particle tracing simulations of unconventional off-axis photoemission geometries in a UEM equipped with a thermionic-emission gun. Specifically, we have explored the impact of experimentally adjustable parameters on the time-of-flight (TOF), the collection efficiency (CE), and the temporal width of ultrashort photoelectron packets. The adjustable parameters include the Wehnelt aperture diameter (DW), the cathode set-back position (Ztip), and the position of the femtosecond laser on the Wehnelt aperture surface relative to the optic axis (Rphoto). Notable findings include significant sensitivity of TOF to DW and Ztip, as well as non-intuitive responses of CE and temporal width to varying Rphoto. As a means to improve accessibility, practical implications and recommendations are emphasized wherever possible.

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光发射几何形状对 4D 超快电子显微镜的时间和效率的影响。
新仪器的开发以及现有技术的不断改进和鉴定,推动了四维超快电子显微镜(UEM)在化学、材料和量子系统研究中的广泛应用。也许是由于进入该领域的门槛仍然很高,激光驱动的四维超快电子显微镜仪器的全部功能仍有待建立,尤其是在极低光束电流(~fA)下运行时。因此,我们着眼于光束的稳定性,在配备热离子发射枪的 UEM 中对非常规离轴光发射几何形状进行了粒子追踪模拟。具体来说,我们探索了实验可调参数对飞行时间(TOF)、收集效率(CE)和超短光电子包时间宽度的影响。可调参数包括韦内特光圈直径(DW)、阴极后退位置(Ztip)以及飞秒激光在韦内特光圈表面相对于光轴的位置(Rphoto)。值得注意的发现包括 TOF 对 DW 和 Ztip 的显著敏感性,以及 CE 和时间宽度对 Rphoto 变化的非直观反应。作为提高可访问性的一种手段,尽可能强调实际意义和建议。
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来源期刊
Chemphyschem
Chemphyschem 化学-物理:原子、分子和化学物理
CiteScore
4.60
自引率
3.40%
发文量
425
审稿时长
1.1 months
期刊介绍: ChemPhysChem is one of the leading chemistry/physics interdisciplinary journals (ISI Impact Factor 2018: 3.077) for physical chemistry and chemical physics. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies. ChemPhysChem is an international source for important primary and critical secondary information across the whole field of physical chemistry and chemical physics. It integrates this wide and flourishing field ranging from Solid State and Soft-Matter Research, Electro- and Photochemistry, Femtochemistry and Nanotechnology, Complex Systems, Single-Molecule Research, Clusters and Colloids, Catalysis and Surface Science, Biophysics and Physical Biochemistry, Atmospheric and Environmental Chemistry, and many more topics. ChemPhysChem is peer-reviewed.
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