Ultrabright Electron Research Articles

Thermodynamic stability and vibrational properties of multi-alkali antimonides

Modern advances in generating ultrabright electron beams have unlocked unprecedented experimental advances based on synchrotron radiation. Current challenges lie in improving the quality of electron sources with novel photocathode materials such as alkali-based semiconductors. To unleash their potential, a detailed characterization and prediction of their fundamental properties is essential. In this work, we employ density functional theory combined with machine learning techniques integrated into the hiphive package to probe the thermodynamic stability of various alkali antimonide crystals, emphasizing the role of the approximations taken for the exchange-correlation potential. Our results reveal that the SCAN functional offers an optimal trade-off between accuracy and computational costs to describe the vibrational properties of these materials. Furthermore, it is found that systems with a higher concentration of Cs atoms exhibit enhanced anharmonicities, which are accurately predicted and characterized with the employed methodology.

Specification and design for full energy beam exploitation of the compact linear accelerator for research and applications

The compact linear accelerator for research and applications (CLARA) is a 250 MeV ultrabright electron beam test facility at STFC Daresbury Laboratory. A user beamline has been designed to maximize the exploitation of CLARA in a variety of fields, including novel acceleration and new modalities of radiotherapy. In this paper, we present the specification and design of this beamline for full energy beam exploitation. We outline the key elements that will provide users access to ultrashort, low emittance electron bunches in two large experiment chambers. The results of start-to-end simulations are reported that verify the expected beam parameters delivered to these chambers. Key technical systems are detailed, including those which facilitate a combination of electron bunches with high-power laser pulses. Published by the American Physical Society 2024

Generation of ultrabright and low energy spread electron beams in laser wakefield acceleration in a uniform plasma

Generation of ultrabright and low energy spread electron beams in laser wakefield acceleration in a uniform plasma

Long range terahertz driven electron acceleration using phase shifters

Terahertz radiation (THz)-based electron acceleration has the potential as a technology for driving the next-generation, compact ultrafast and ultrabright electron and x-ray sources. Dephasing is one of the key problems that prevent long THz–electron interaction lengths in the sub- to few-MeV range, where electron velocities vary significantly during high-field acceleration. Here, we present a phase-shifter design with double vacuum channels to alternate the phase velocity that effectively extends the THz–electron interaction length in THz-powered dielectrically loaded waveguides. The electrons are swept multiple-times back and forth through the accelerating phase of the THz wave to undergo continuous acceleration along the entire interaction. In addition, the double vacuum channel design enables increases in both the phase and group velocities of the THz wave, which leads to an adaptive synchronous acceleration with extended interaction length. This method paves the way for the practical implementation of THz-powered devices for high-energy ultrafast electron sources.

Highly efficient nonlinear optical emission from a subwavelength crystalline silicon cuboid mediated by supercavity mode

The low quantum efficiency of silicon (Si) has been a long-standing challenge for scientists. Although improvement of quantum efficiency has been achieved in porous Si or Si quantum dots, highly efficient Si-based light sources prepared by using the current fabrication technooloy of Si chips are still being pursued. Here, we proposed a strategy, which exploits the intrinsic excitation of carriers at high temperatures, to modify the carrier dynamics in Si nanoparticles. We designed a Si/SiO2 cuboid supporting a quasi-bound state in the continuum (quasi-BIC) and demonstrated the injection of dense electron-hole plasma via two-photon-induced absorption by resonantly exciting the quasi-BIC with femtosecond laser pulses. We observed a significant improvement in quantum efficiency by six orders of magnitude to ~13%, which is manifested in the ultra-bright hot electron luminescence emitted from the Si/SiO2 cuboid. We revealed that femtosecond laser light with transverse electric polarization (i.e., the electric field perpendicular to the length of a Si/SiO2 cuboid) is more efficient for generating hot electron luminescence in Si/SiO2 cuboids as compared with that of transverse magnetic polarization (i.e., the magnetic field perpendicular to the length of a Si/SiO2 cuboid). Our findings pave the way for realizing on-chip nanoscale Si light sources for photonic integrated circuits and open a new avenue for manipulating the luminescence properties of semiconductors with indirect bandgaps.

Ultrafast Imaging of Molecular Dynamics Using Ultrafast Low-Frequency Lasers, X-ray Free Electron Lasers, and Electron Pulses.

The requirement of high space-time resolution and brightness is a great challenge for imaging atomic motion and making molecular movies. Important breakthroughs in ultrabright tabletop laser, X-ray, and electron sources have enabled the direct imaging of evolving molecular structures in chemical processes, and recent experimental advances in preparing ultrafast laser and electron pulses resulted in molecular imaging with femtosecond time resolution. This Perspective presents an overview of the versatile imaging methods of molecular dynamics. High-order harmonic generation imaging and photoelectron diffraction imaging are based on laser-induced ionization and rescattering processes. Coulomb explosion imaging retrieves molecular structural information by detecting the momentum vectors of fragmented ions. Diffraction imaging encodes molecular structural and electronic information in reciprocal space. We also present various applications of these ultrafast imaging methods in resolving laser-induced nuclear and electronic dynamics.

Ab Initio Quantum-Mechanical Predictions of Semiconducting Photocathode Materials.

Ab initio Quantum-Mechanical methods are well-established tools for material characterization and discovery in many technological areas. Recently, state-of-the-art approaches based on density-functional theory and many-body perturbation theory were successfully applied to semiconducting alkali antimonides and tellurides, which are currently employed as photocathodes in particle accelerator facilities. The results of these studies have unveiled the potential of ab initio methods to complement experimental and technical efforts for the development of new, more efficient materials for vacuum electron sources. Concomitantly, these findings have revealed the need for theory to go beyond the status quo in order to face the challenges of modeling such complex systems and their properties in operando conditions. In this review, we summarize recent progress in the application of ab initio many-body methods to investigate photocathode materials, analyzing the merits and the limitations of the standard approaches with respect to the confronted scientific questions. In particular, we emphasize the necessary trade-off between computational accuracy and feasibility that is intrinsic to these studies, and propose possible routes to optimize it. We finally discuss novel schemes for computationally-aided material discovery that are suitable for the development of ultra-bright electron sources toward the incoming era of artificial intelligence.

Mapping Atomic Motions with Ultrabright Electrons: Fundamental Space-Time Limits to Imaging Chemistry and Biological Processes

Mapping Atomic Motions with Ultrabright Electrons: Fundamental Space-Time Limits to Imaging Chemistry and Biological Processes

Design of ultrabright 270 keV DC photoelectron gun for ultrafast electron diffraction

Compact DC photoelectron guns of high-voltage are highly desired to output ultrabright and ultrashort electron pulses for accessing irreversible processes by using the ultrafast electron diffraction (UED) technique. The high-voltage breakdown, however, is a major technical barrier to providing an intense electric field strength in a condensed space between the photocathode and the anode when the voltage is over 120 kV. In this work, by adopting the concept of voltage division, we propose a novel design of ultrabright near-relativistic DC photoelectron guns for UED. The electric field breakdown mainly caused by micro-particle collision could be avoided such that an optimized three-level acceleration DC gun can work with an electron energy of up to 270 keV and an electric field strength of up to 15 MV/m. N-particle simulations of the electron pulse propagation show that, with such a DC electron gun, it is possible to have ultrabright and ultrashort electron probe pulses with no jitter issue.

Design, specifications, and first beam measurements of the compact linear accelerator for research and applications front end

The compact linear accelerator for research and applications (CLARA) is an ultrabright electron beam test facility being developed at STFC Daresbury Laboratory. The ultimate aim of CLARA is to test advanced free electron laser (FEL) schemes that can later be implemented on existing and future short-wavelength FELs. In addition, CLARA is a unique facility to provide a high-quality electron beam to test novel concepts and ideas in a wide range of disciplines and to function as a technology demonstrator for a future United Kingdom x-ray FEL facility. CLARA is being built in three phases; the first phase, or front end (FE), comprises an S-band rf photoinjector, a linac, and an S-bend merging with the existing versatile electron linear accelerator beam line; the second phase will complete the acceleration to full beam energy of 250 MeV and also incorporate a separate beam line for use of electrons at 250 MeV; and the third phase will include the FEL section. The CLARA FE was commissioned during 2018, and the facility was later made available for user experiments. Significant advancements have been made in developing high-level software and a simulation framework for start-to-end simulations. The high-level software has been successfully used for unmanned rf conditioning and for characterization of the electron beam. This paper describes the design of the CLARA FE, performance of technical systems, high-level software developments, preliminary results of measured beam parameters, and plans for improvements and upgrades. © 2020 authors. Published by the American Physical Society.

Mapping Atomic Motions with Electrons: Toward the Quantum Limit to Imaging Chemistry

Recent advances in ultrafast electron and X-ray diffraction have pushed imaging of structural dynamics into the femtosecond time domain, that is, the fundamental time scale of atomic motion. New physics can be reached beyond the scope of traditional diffraction or reciprocal space imaging. By exploiting the high time resolution, it has been possible to directly observe the collapse of nearly innumerable possible nuclear motions to a few key reaction modes that direct chemistry. It is this reduction in dimensionality in the transition state region that makes chemistry a transferable concept, with the same class of reactions being applicable to synthetic strategies to nearly arbitrary levels of complexity. The ability to image the underlying key reaction modes has been achieved with resolution to relative changes in atomic positions to better than 0.01 Å, that is, comparable to thermal motions. We have effectively reached the fundamental space-time limit with respect to the reaction energetics and imaging the acting forces. In the process of ensemble measured structural changes, we have missed the quantum aspects of chemistry. This perspective reviews the current state of the art in imaging chemistry in action and poses the challenge to access quantum information on the dynamics. There is the possibility with the present ultrabright electron and X-ray sources, at least in principle, to do tomographic reconstruction of quantum states in the form of a Wigner function and density matrix for the vibrational, rotational, and electronic degrees of freedom. Accessing this quantum information constitutes the ultimate demand on the spatial and temporal resolution of reciprocal space imaging of chemistry. Given the much shorter wavelength and corresponding intrinsically higher spatial resolution of current electron sources over X-rays, this Perspective will focus on electrons to provide an overview of the challenge on both the theory and the experimental fronts to extract the quantum aspects of molecular dynamics.

Electronic structure and core electron fingerprints of caesium-based multi-alkali antimonides for ultra-bright electron sources

The development of novel photocathode materials for ultra-bright electron sources demands efficient and cost-effective strategies that provide insight and understanding of the intrinsic material properties given the constraints of growth and operational conditions. To address this question, we propose a viable way to establish correlations between calculated and measured data on core electronic states of Cs-K-Sb materials. To do so, we combine first-principles calculations based on all-electron density-functional theory on the three alkali antimonides Cs3Sb, Cs2KSb, and CsK2Sb with x-ray photoemission spectroscopy (XPS) on Cs-K-Sb photocathode samples. Within the GW approximation of many-body perturbation theory, we obtain quantitative predictions of the band gaps of these materials, which range from 0.57 eV in Cs2KSb to 1.62 eV in CsK2Sb and manifest direct or indirect character depending on the relative potassium content. Our theoretical electronic-structure analysis also reveals that the core states of these systems have binding energies that depend only on the atomic species and their crystallographic sites, with largest shifts of the order of 2 eV and 0.5 eV associated to K 2p and Sb 3d states, respectively. This information can be correlated to the maxima in the XPS survey spectra, where such peaks are clearly visible. In this way, core-level shifts can be used as fingerprints to identify specific compositions of Cs-K-Sb materials and their relation with the measured values of quantum efficiency. Our results represent the first step towards establishing a robust connection between the experimental preparation and characterization of photocathodes, the ab initio prediction of their electronic structure, and the modeling of emission and beam formation processes.

Mapping Atomic Motions with Ultrabright Electrons: Fundamental Space-Time Limits to Imaging Chemistry and Biological Processes

Mapping Atomic Motions with Ultrabright Electrons: Fundamental Space-Time Limits to Imaging Chemistry and Biological Processes

First-principles many-body study of the electronic and optical properties of CsK2Sb, a semiconducting material for ultra-bright electron sources

We present a comprehensive first-principles investigation of the electronic and optical properties of CsK2Sb, a semiconducting material for ultra-bright electron sources for particle accelerators. Our study, based on density-functional theory and many-body perturbation theory, provides all the ingredients to model the emission of this material as a photocathode, including band gap, band dispersion, and optical absorption. An accurate description of these properties beyond the mean-field picture is relevant to take into account many-body effects. We discuss our results in the context of state-of-the-art electron sources for particle accelerators to set the stage towards improved modeling of quantum efficiency, intrinsic emittance, and other relevant quantities determining the macroscopic characteristics of photocathodes for ultra-bright beams.

Optically controlled laser–plasma electron accelerator for compact gamma-ray sources

Generating quasi-monochromatic, femtosecond γ-ray pulses via Thomson scattering (TS) demands exceptional electron beam (e-beam) quality, such as percent-scale energy spread and five-dimensional brightness over 1016 A m–2. We show that near-GeV e-beams with these metrics can be accelerated in a cavity of electron density, driven with an incoherent stack of Joule-scale laser pulses through a mm-size, dense plasma (n0 ∼ 1019 cm−3). Changing the time delay, frequency difference, and energy ratio of the stack components controls the e-beam phase space on the femtosecond scale, while the modest energy of the optical driver helps afford kHz-scale repetition rate at manageable average power. Blue-shifting one stack component by a considerable fraction of the carrier frequency makes the stack immune to self-compression. This, in turn, minimizes uncontrolled variation in the cavity shape, suppressing continuous injection of ambient plasma electrons, preserving a single, ultra-bright electron bunch. In addition, weak focusing of the trailing component of the stack induces periodic injection, generating, in a single shot, a train of bunches with controllable energy spacing and femtosecond synchronization. These designer e-beams, inaccessible to conventional acceleration methods, generate, via TS, gigawatt γ-ray pulses (or multi-color pulse trains) with the mean energy in the range of interest for nuclear photonics (4–16 MeV), containing over 106 photons within a microsteradian-scale observation cone.

An ultrabright and monochromatic electron point source made of a LaB6 nanowire.

Electron sources in the form of one-dimensional nanotubes and nanowires are an essential tool for investigations in a variety of fields, such as X-ray computed tomography, flexible displays, chemical sensors and electron optics applications. However, field emission instability and the need to work under high-vacuum or high-temperature conditions have imposed stringent requirements that are currently limiting the range of application of electron sources. Here we report the fabrication of a LaB6 nanowire with only a few La atoms bonded on the tip that emits collimated electrons from a single point with high monochromaticity. The nanostructured tip has a low work function of 2.07 eV (lower than that of Cs) while remaining chemically inert, two properties usually regarded as mutually exclusive. Installed in a scanning electron microscope (SEM) field emission gun, our tip shows a current density gain that is about 1,000 times greater than that achievable with W(310) tips, and no emission decay for tens of hours of operation. Using this new SEM, we acquired very low-noise, high-resolution images together with rapid chemical compositional mapping using a tip operated at room temperature and at 10-times higher residual gas pressure than that required for W tips.

Transverse profile imager for ultrabright electron beams

A transverse profile imager for ultrabright electron beams is presented, which overcomes resolution issues in present designs by observing the Scheimpflug imaging condition as well as the Snell-Descartes law of refraction in the scintillating crystal. Coherent optical transition radiation emitted by highly compressed electron bunches on the surface of the crystal is directed away from the camera, allowing to use the monitor for profile measurements of electron bunches suitable for X-ray free electron lasers. The optical design has been verified by ray tracing simulations, and the angular dependency of the resolution has been verified experimentally. An instrument according to the presented design principles has been used in the SwissFEL Injector Test Facility, and different scintillator materials have been tested. Measurements in conjunction with a transverse deflecting radiofrequency structure and an array of quadrupole magnets demonstrate a normalized slice emittance of 25 nm in the core of a 30 fC electron beam at a pulse length of 10 ps and a particle energy of 230 MeV.

Nitrogen plasma formation through terahertz-induced ultrafast electron field emission

Electron microscopy and electron diffraction techniques rely on electron sources. Those sources require strong electric fields to extract electrons from metals, either by the photoelectric effect, driven by multiphoton absorption of strong laser fields, or in the static field emission regime. Terahertz (THz) radiation, commonly understood to be nonionizing due to its low photon energy, is here shown to produce electron field emission. We demonstrate that a carrier-envelope phase-stable single-cycle optical field at THz frequencies interacting with a metallic microantenna can generate and accelerate ultrashort and ultrabright electron bunches into free space, and we use these electrons to excite and ionize ambient nitrogen molecules near the antenna. The associated UV emission from the gas forms a novel THz wave detector, which, in contrast with conventional photon-counting or heat-sensitive devices, is ungated and sensitive to the peak electric field in a strongly nonlinear fashion.

Mapping atomic motions with ultrabright electrons: towards fundamental limits in space-time resolution.

The long held objective of directly observing atomic motions during the defining moments of chemistry has been achieved based on ultrabright electron sources that have given rise to a new field of atomically resolved structural dynamics. This class of experiments requires not only simultaneous sub-atomic spatial resolution with temporal resolution on the 100 femtosecond time scale but also has brightness requirements approaching single shot atomic resolution conditions. The brightness condition is in recognition that chemistry leads generally to irreversible changes in structure during the experimental conditions and that the nanoscale thin samples needed for electron structural probes pose upper limits to the available sample or "film" for atomic movies. Even in the case of reversible systems, the degree of excitation and thermal effects require the brightest sources possible for a given space-time resolution to observe the structural changes above background. Further progress in the field, particularly to the study of biological systems and solution reaction chemistry, requires increased brightness and spatial coherence, as well as an ability to tune the electron scattering cross-section to meet sample constraints. The electron bunch density or intensity depends directly on the magnitude of the extraction field for photoemitted electron sources and electron energy distribution in the transverse and longitudinal planes of electron propagation. This work examines the fundamental limits to optimizing these parameters based on relativistic electron sources using re-bunching cavity concepts that are now capable of achieving 10 femtosecond time scale resolution to capture the fastest nuclear motions. This analysis is given for both diffraction and real space imaging of structural dynamics in which there are several orders of magnitude higher space-time resolution with diffraction methods. The first experimental results from the Relativistic Electron Gun for Atomic Exploration (REGAE) are given that show the significantly reduced multiple electron scattering problem in this regime, which opens up micron scale systems, notably solution phase chemistry, to atomically resolved structural dynamics.

Nanostructured ultrafast silicon-tip optical field-emitter arrays.

Femtosecond ultrabright electron sources with spatially structured emission are an enabling technology for free-electron lasers, compact coherent X-ray sources, electron diffractive imaging, and attosecond science. In this work, we report the design, modeling, fabrication, and experimental characterization of a novel ultrafast optical field emission cathode comprised of a large (>100,000 tips), dense (4.6 million tips·cm(-2)), and highly uniform (<1 nm tip radius deviation) array of nanosharp high-aspect-ratio silicon columns. Such field emitters offer an attractive alternative to UV photocathodes while providing a direct means of structuring the emitted electron beam. Detailed measurements and simulations show pC electron bunches can be generated in the multiphoton and tunneling regime within a single optical cycle, enabling significant advances in electron diffractive imaging and coherent X-ray sources on a subfemtosecond time scale, not possible before. At high charge emission yields, a slow rollover in charge is explained as a combination of the onset of tunneling emission and the formation of a virtual cathode.