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1. Single-photoelectron collection efficiency in 4D ultrafast electron microscopy

   https://doi.org/10.1039/d2cp01250b  

   Curtis, Wyatt A.; Willis, Simon A.; Flannigan, David J. (June 2022, Physical Chemistry Chemical Physics)

   In femtosecond (fs) 4D ultrafast electron microscopy (UEM), a tradeoff is made between photoelectrons per packet and time resolution. One consequence of this can be longer-than-desirable acquisition times for low-density packets, and particularly for low repetition rates when complete photothermal dissipation is required. Thus, gaining an understanding of photoelectron trajectories in the gun region is important for identifying factors that limit collection efficiency (CE; fraction of photoelectrons that enter the illumination system). Here, we continue our work on the systematic study of photoelectron trajectories in the gun region of a Thermo Fisher/FEI Tecnai Femto UEM, focusing specifically on CE in the single-electron regime. Using General Particle Tracer, calculated field maps, and the exact architecture of the Tecnai Femto UEM, we simulated the effects of fs laser parameters and key gun elements on CE. The results indicate CE strongly depends upon the laser spot size on the source, the (unbiased) Wehnelt aperture diameter, and the incident photon energy. The CE dispersion with laser spot size is found to be strongly dependent on aperture diameter, being nearly dispersionless for the largest apertures. A gun crossover is also observed, with the beam-waist position being dependent on the aperture diameter, further illustrating that the Wehnelt aperture acts as a simple, fixed electrostatic lens in UEM mode. This work provides further insights into the operational aspects of fs 4D UEM. 

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2. Delineation of the impact on temporal behaviors of off-axis photoemission in an ultrafast electron microscope

   https://doi.org/10.1063/5.0222993  

   Chen, Jialiang; Willis, Simon A; Flannigan, David J (September 2024, Review of Scientific Instruments)

   Efforts to push the spatiotemporal imaging-resolution limits of femtosecond laser-driven ultrafast electron microscopes (UEMs) to the combined angstrom–fs range will benefit from stable sources capable of generating high bunch charges. Recent demonstrations of unconventional off-axis photoemitting geometries are promising, but connections to the observed onset of structural dynamics are yet to be established. Here we use the in-situ photoexcitation of coherent phonons to quantify the relative time-of-flight (r-TOF) of photoelectron packets generated from the Ni Wehnelt aperture and from a Ta cathode set-back from the aperture plane. We further support the UEM experiments with particle-tracing simulations of the precise electron-gun architecture and photoemitting geometries. In this way, we measure discernible shifts in electron-packet TOF of tens of picoseconds for the two photoemitting surfaces. These shifts arise from the impact that the Wehnelt-aperture off-axis orientation has on the electron-momentum distribution, which modifies both the collection efficiency and the temporal-packet distribution relative to on-axis emission. Future needs are identified; we expect this and other developments in UEM electron-gun configuration to expand the range of material phenomena that can be directly imaged on scales commensurate with fundamental structural dynamics. 

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3. Wehnelt photoemission in an ultrafast electron microscope: Stability and usability

   https://doi.org/10.1063/5.0214246  

   Willis, Simon A; Curtis, Wyatt A; Flannigan, David J (July 2024, Journal of Applied Physics)

   We tested and compared the stability and usability of three different cathode materials and configurations in a thermionic-based ultrafast electron microscope: (1) on-axis thermionic and photoemission from a custom 100 μm diameter LaB6 source with a graphite guard ring, (2) off-axis photoemission from the Ni aperture surface of the Wehnelt electrode, and (3) on-axis thermionic and photoemission from a custom 200 μm diameter polycrystalline Ta source. For each cathode type and configuration, including the Ni Wehnelt aperture, we illustrate how the photoelectron beam-current stability is deleteriously impacted by simultaneous cooling of the source following thermionic heating. Furthermore, we demonstrate usability via collection of parallel- and convergent-beam electron diffraction patterns and by formation of the optimum probe size. We find that usability of the off-axis Ni Wehnelt-aperture photoemission is at least comparable to on-axis LaB6 thermionic emission, as well as to on-axis photoemission [the heretofore conventional approach to ultrafast electron microscopy (UEM) in thermionic-based instruments]. However, the stability and achievable beam currents for off-axis photoemission from the Wehnelt aperture were superior to that of the other cathode types and configurations, regardless of the electron-emission mechanism. Beam-current stability for this configuration was found to be ±1% (one standard deviation from the mean) for 70 min (longest duration tested), and steady-state beam current was reached within the sampling-time resolution used here (∼1 s) for 15 pA beam currents (i.e., 460 electrons per packet for a 200 kHz repetition rate). Repeatability and robustness of the steady-state condition were also found to be within ±1% of the mean. We discuss the implications of these findings for UEM imaging and diffraction experiments, for pulsed-beam damage measurements, and for practical switching between optimum conventional TEM and UEM operation within the same instrument. 

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4. Toward Å–fs–meV resolution in electron microscopy: systematic simulation of the temporal spread of single-electron packets

   https://doi.org/10.1039/d1cp03518e  

   Curtis, Wyatt A.; Flannigan, David J. (October 2021, Physical Chemistry Chemical Physics)

   Though efforts to improve the temporal resolution of transmission electron microscopes (TEMs) have waxed and waned for decades, with relatively recent advances routinely reaching sub-picosecond scales, fundamental and practical challenges have hindered the advance of combined Å–fs–meV resolutions, particularly for core-loss spectroscopy and real-space imaging. This is due in no small part to the complexity of the approach required to access timescales upon which electrons, atoms, molecules, and materials first begin to respond and transform – attoseconds to picoseconds. Here we present part of a larger effort devoted to systematically mapping the instrument parameter space of a TEM modified to reach ultrafast timescales. With General Particle Tracer, we studied the statistical temporal distributions of single-electron packets as a function of various fs pulsed-laser parameters and electron-gun configurations and fields for the exact architecture and dimensions of a Thermo Fisher Tecnai Femto ultrafast electron microscope. We focused on easily-adjustable parameters, such as laser pulse duration, laser spot size, photon energy, Wehnelt aperture diameter, and photocathode size. In addition to establishing trends and dispersion behaviors, we identify regimes within which packet duration can be 100s of fs and approach the 300 fs laser limit employed here. Overall, the results provide a detailed picture of the temporal behavior of single-electron packets in the Tecnai Femto gun region, forming the initial contribution of a larger effort. 

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5. The Redshift Evolution of the Binary Black Hole Merger Rate: A Weighty Matter

   https://doi.org/10.3847/1538-4357/ac64a3  

   van Son, L. A. C.; de Mink, S. E.; Callister, T.; Justham, S.; Renzo, M.; Wagg, T.; Broekgaarden, F. S.; Kummer, F.; Pakmor, R.; Mandel, I. (May 2022, The Astrophysical Journal)

   Abstract Gravitational-wave detectors are starting to reveal the redshift evolution of the binary black hole (BBH) merger rate,R_BBH(z). We make predictions forR_BBH(z) as a function of black hole mass for systems originating from isolated binaries. To this end, we investigate correlations between the delay time and black hole mass by means of the suite of binary population synthesis simulations,COMPAS. We distinguish two channels: the common envelope (CE), and the stable Roche-lobe overflow (RLOF) channel, characterized by whether the system has experienced a common envelope or not. We find that the CE channel preferentially produces BHs with masses below about 30M_⊙and short delay times (t_delay≲ 1 Gyr), while the stable RLOF channel primarily forms systems with BH masses above 30M_⊙and long delay times (t_delay≳ 1 Gyr). We provide a new fit for the metallicity-dependent specific star formation rate density based on the Illustris TNG simulations, and use this to convert the delay time distributions into a prediction ofR_BBH(z). This leads to a distinct redshift evolution ofR_BBH(z) for high and low primary BH masses. We furthermore find that, at high redshift,R_BBH(z) is dominated by the CE channel, while at low redshift, it contains a large contribution (∼40%) from the stable RLOF channel. Our results predict that, for increasing redshifts, BBHs with component masses above 30M_⊙will become increasingly scarce relative to less massive BBH systems. Evidence of this distinct evolution ofR_BBH(z) for different BH masses can be tested with future detectors. 

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