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

Willis, Simon A.; Flannigan, David J.

doi:10.1002/cphc.202401032

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

Journal Article · 12 January 2025 · ChemPhysChem

DOI: https://doi.org/10.1002/cphc.202401032 · OSTI ID:2507255

Willis, Simon A. ^[1]; Flannigan, David J. ^[1]

University of Minnesota, Minneapolis, MN (United States)

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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Research Organization:: University of Minnesota, Minneapolis, MN (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: SC0023708

OSTI ID:: 2507255

Journal Information:: ChemPhysChem, Journal Name: ChemPhysChem Journal Issue: 5 Vol. 26; ISSN 1439-4235

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

References (39)

Design and implementation of a fs-resolved transmission electron microscope based on thermionic gun technology Piazza, L.; Masiel, D. J.; LaGrange, T. Chemical Physics, Vol. 423 https://doi.org/10.1016/j.chemphys.2013.06.026	journal	September 2013
Ultrafast electron microscopy: Instrument response from the single-electron to high bunch-charge regimes Plemmons, Dayne A.; Flannigan, David J. Chemical Physics Letters, Vol. 683 https://doi.org/10.1016/j.cplett.2017.01.055	journal	September 2017
Pulsed-beam transmission electron microscopy and radiation damage Flannigan, David J.; VandenBussche, Elisah J. Micron, Vol. 172 https://doi.org/10.1016/j.micron.2023.103501	journal	September 2023
Electron beam dynamics in an ultrafast transmission electron microscope with Wehnelt electrode Bücker, K.; Picher, M.; Crégut, O. Ultramicroscopy, Vol. 171 https://doi.org/10.1016/j.ultramic.2016.08.014	journal	December 2016
Ultrafast transmission electron microscopy using a laser-driven field emitter: Femtosecond resolution with a high coherence electron beam Feist, Armin; Bach, Nora; Rubiano da Silva, Nara Ultramicroscopy, Vol. 176 https://doi.org/10.1016/j.ultramic.2016.12.005	journal	May 2017
Development of a high brightness ultrafast Transmission Electron Microscope based on a laser-driven cold field emission source Houdellier, F.; Caruso, G. M.; Weber, S. Ultramicroscopy, Vol. 186 https://doi.org/10.1016/j.ultramic.2017.12.015	journal	March 2018
Coherent Phonon Disruption and Lock-In during a Photoinduced Charge-Density-Wave Phase Transition Reisbick, Spencer A.; Zhang, Yichao; Chen, Jialiang The Journal of Physical Chemistry Letters, Vol. 12, Issue 27 https://doi.org/10.1021/acs.jpclett.1c01673	journal	July 2021
Imaging Nanometer Phonon Softening at Crystal Surface Steps with 4D Ultrafast Electron Microscopy Zhang, Yichao; Flannigan, David J. Nano Letters, Vol. 21, Issue 17 https://doi.org/10.1021/acs.nanolett.1c02524	journal	August 2021
Ultrafast Nanoimaging of Spin-Mediated Shear Waves in an Acoustic Cavity Zhou, Faran; Liu, Haihua; Zajac, Marc Nano Letters, Vol. 23, Issue 22, p. 10213-10220 https://doi.org/10.1021/acs.nanolett.3c02747	journal	November 2023
Reducing Radiation Damage in Soft Matter with Femtosecond-Timed Single-Electron Packets VandenBussche, Elisah J.; Flannigan, David J. Nano Letters, Vol. 19, Issue 9 https://doi.org/10.1021/acs.nanolett.9b03074	journal	August 2019
Ultrafast Electron Microscopy of Nanoscale Charge Dynamics in Semiconductors Yannai, Michael; Dahan, Raphael; Gorlach, Alexey ACS Nano, Vol. 17, Issue 4 https://doi.org/10.1021/acsnano.2c10481	journal	February 2023
Charge Dynamics Electron Microscopy: Nanoscale Imaging of Femtosecond Plasma Dynamics Madan, Ivan; Dias, Eduardo J. C.; Gargiulo, Simone ACS Nano, Vol. 17, Issue 4 https://doi.org/10.1021/acsnano.2c10482	journal	February 2023
Mitigating Damage to Hybrid Perovskites Using Pulsed-Beam TEM VandenBussche, Elisah J.; Clark, Catherine P.; Holmes, Russell J. ACS Omega, Vol. 5, Issue 49 https://doi.org/10.1021/acsomega.0c04711	journal	December 2020
Atomic-Scale Imaging in Real and Energy Space Developed in Ultrafast Electron Microscopy Park, Hyun Soon; Baskin, J. Spencer; Kwon, Oh-Hoon Nano Letters, Vol. 7, Issue 9 https://doi.org/10.1021/nl071369q	journal	September 2007
Photon-induced near-field electron microscopy Barwick, Brett; Flannigan, David J.; Zewail, Ahmed H. Nature, Vol. 462, Issue 7275 https://doi.org/10.1038/nature08662	journal	December 2009
Quantum coherent optical phase modulation in an ultrafast transmission electron microscope Feist, Armin; Echternkamp, Katharina E.; Schauss, Jakob Nature, Vol. 521, Issue 7551 https://doi.org/10.1038/nature14463	journal	May 2015
Femtosecond electron imaging of defect-modulated phonon dynamics Cremons, Daniel R.; Plemmons, Dayne A.; Flannigan, David J. Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms11230	journal	April 2016
High-temporal-resolution electron microscopy for imaging ultrafast electron dynamics Hassan, M. Th.; Baskin, J. S.; Liao, B. Nature Photonics, Vol. 11, Issue 7 https://doi.org/10.1038/nphoton.2017.79	journal	May 2017
Ramsey-type phase control of free-electron beams Echternkamp, Katharina E.; Feist, Armin; Schäfer, Sascha Nature Physics, Vol. 12, Issue 11 https://doi.org/10.1038/nphys3844	journal	August 2016
Lorentz microscopy of optical fields Gaida, John H.; Lourenço-Martins, Hugo; Yalunin, Sergey V. Nature Communications, Vol. 14, Issue 1 https://doi.org/10.1038/s41467-023-42054-3	journal	October 2023
Attosecond electron pulse trains and quantum state reconstruction in ultrafast transmission electron microscopy Priebe, Katharina E.; Rathje, Christopher; Yalunin, Sergey V. Nature Photonics, Vol. 11, Issue 12 https://doi.org/10.1038/s41566-017-0045-8	journal	November 2017
Attosecond electron microscopy by free-electron homodyne detection Gaida, John H.; Lourenço-Martins, Hugo; Sivis, Murat Nature Photonics, Vol. 18, Issue 5 https://doi.org/10.1038/s41566-024-01380-8	journal	February 2024
Diffraction and microscopy with attosecond electron pulse trains Morimoto, Yuya; Baum, Peter Nature Physics, Vol. 14, Issue 3 https://doi.org/10.1038/s41567-017-0007-6	journal	November 2017
Controlling free electrons with optical whispering-gallery modes Kfir, Ofer; Lourenço-Martins, Hugo; Storeck, Gero Nature, Vol. 582, Issue 7810 https://doi.org/10.1038/s41586-020-2320-y	journal	June 2020
Toward Å–fs–meV resolution in electron microscopy: systematic simulation of the temporal spread of single-electron packets Curtis, Wyatt A.; Flannigan, David J. Physical Chemistry Chemical Physics, Vol. 23, Issue 41 https://doi.org/10.1039/D1CP03518E	journal	January 2021
Single-photoelectron collection efficiency in 4D ultrafast electron microscopy Curtis, Wyatt A.; Willis, Simon A.; Flannigan, David J. Physical Chemistry Chemical Physics, Vol. 24, Issue 22 https://doi.org/10.1039/D2CP01250B	journal	January 2022
Ultrashort electron pulses for diffraction, crystallography and microscopy: theoretical and experimental resolutions Gahlmann, Andreas; Tae Park, Sang; Zewail, Ahmed H. Physical Chemistry Chemical Physics, Vol. 10, Issue 20 https://doi.org/10.1039/b802136h	journal	January 2008
Femtosecond electron pulse propagation for ultrafast electron diffraction Reed, Bryan W. Journal of Applied Physics, Vol. 100, Issue 3 https://doi.org/10.1063/1.2227710	journal	August 2006
Communication: Effects of thermionic-gun parameters on operating modes in ultrafast electron microscopy Kieft, Erik; Schliep, Karl B.; Suri, Pranav K. Structural Dynamics, Vol. 2, Issue 5 https://doi.org/10.1063/1.4930174	journal	September 2015
Influence of cathode geometry on electron dynamics in an ultrafast electron microscope Ji, Shaozheng; Piazza, Luca; Cao, Gaolong Structural Dynamics, Vol. 4, Issue 5 https://doi.org/10.1063/1.4994004	journal	September 2017
Characterization of a time-resolved electron microscope with a Schottky field emission gun Olshin, Pavel K.; Drabbels, Marcel; Lorenz, Ulrich J. Structural Dynamics, Vol. 7, Issue 5 https://doi.org/10.1063/4.0000034	journal	September 2020
Characterization of a LaB6 tip as a thermionically enhanced photoemitter Guo, Xuefei; Chaudhuri, Dipanjan; Bielinski, Nina Applied Physics Letters, Vol. 124, Issue 1 https://doi.org/10.1063/5.0179354	journal	January 2024
Wehnelt photoemission in an ultrafast electron microscope: Stability and usability Willis, Simon A.; Curtis, Wyatt A.; Flannigan, David J. Journal of Applied Physics, Vol. 136, Issue 2 https://doi.org/10.1063/5.0214246	journal	July 2024
Delineation of the impact on temporal behaviors of off-axis photoemission in an ultrafast electron microscope Chen, Jialiang; Willis, Simon A.; Flannigan, David J. Review of Scientific Instruments, Vol. 95, Issue 9 https://doi.org/10.1063/5.0222993	journal	September 2024
Four-dimensional ultrafast electron microscopy Lobastov, V. A.; Srinivasan, R.; Zewail, A. H. Proceedings of the National Academy of Sciences, Vol. 102, Issue 20 https://doi.org/10.1073/pnas.0502607102	journal	May 2005
Attomicroscopy: from femtosecond to attosecond electron microscopy Hassan, Mohammed Th Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 51, Issue 3 https://doi.org/10.1088/1361-6455/aaa183	journal	January 2018
Chirped imaging pulses in four-dimensional electron microscopy: femtosecond pulsed hole burning Park, Sang Tae; Kwon, Oh-Hoon; Zewail, Ahmed H. New Journal of Physics, Vol. 14, Issue 5 https://doi.org/10.1088/1367-2630/14/5/053046	journal	May 2012
Imaging coherent phonons and precursor dynamics in LaFeAsO with 4D ultrafast electron microscopy Gnabasik, Ryan A.; Suri, Pranav K.; Chen, Jialiang Physical Review Materials, Vol. 6, Issue 2 https://doi.org/10.1103/PhysRevMaterials.6.024802	journal	February 2022
Femtosecond-resolved imaging of a single-particle phase transition in energy-filtered ultrafast electron microscopy Kim, Ye-Jin; Nho, Hak-Won; Ji, Shaozheng Science Advances, Vol. 9, Issue 4 https://doi.org/10.1126/sciadv.add5375	journal	January 2023

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