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Alkali antimonides are well established as high efficiency, low intrinsic emittance photocathodes for accelerators and photon detectors. However, conventionally grown alkali antimonide films are polycrystalline with surface disorder and roughness that can limit achievable beam brightness. Ordering the crystalline structure of alkali antimonides has the potential to deliver higher brightness electron beams by reducing surface disorder and enabling the engineering of material properties at the level of atomic layers. In this report, we demonstrate the growth of ordered Cs$_{3}$Sb films on single crystal substrates 3C-SiC and graphene-coated 4H-SiC using pulsed laser deposition and conventional thermal evaporation growth techniques. The crystalline structures of the Cs$_{3}$Sb films were examined using reflection high energy electron diffraction (RHEED) and X-ray diffraction (XRD) diagnostics, while film thickness and roughness estimates were made using x-ray reflectivity (XRR). With these tools, we observed ordered domains in less than 10 nm thick films with quantum efficiencies greater than one percent at 530 nm. Moreover, we identify structural features such as Laue oscillations indicative of highly ordered films. We found that Cs$_{3}$Sb films grew with flat, fiber-textured surfaces on 3C-SiC and with multiple ordered domains and sub-nanometer surface roughness on graphene-coated 4H-SiC under our growth conditions. We identify the crystallographic orientations of Cs$_{3}$Sb grown on graphene-coated 4H-SiC substrates and discuss the significance of examining the crystal structure of these films for growing epitaxial heterostructures in future experiments.

Spin-polarized photoemission from wurtzite and zinc-blende gallium nitride (GaN) photocathodes has been observed and measured for the first time. The p-doped GaN photocathodes were epitaxially grown and activated to negative electron affinity (NEA) with a cesium monolayer deposited on their surfaces. A field-retarding Mott polarimeter was used to measure the spin-polarization of electrons photoemitted from the top of the valence band. A spectral scan with a tunable optical parametric amplifier (OPA) constructed to provide low-bandwidth light revealed peak spin polarizations of 17% and 29% in the wurtzite and zinc-blende photocathodes, respectively. Zinc-blende GaN results are analyzed with a spin-polarization model accounting for experimental parameters used in the measurements, while possible mechanisms influencing the obtained spin polarization values of wurtzite GaN are discussed.

Achieving maximum electron beam brightness in photoinjectors requires detailed control of the 3D bunch shape and precise tuning of the beam focusing. Even in state-of-the-art designs, slice emittance growth due to nonlinear space charge forces and partial nonlaminarity often remains non-negligible. In this work we introduce a new means to linearize the transverse slice phase space: a sacrificial portion of the bunch's own charge distribution, formed into a wavebroken shock front by highly nonlinear space charge forces within the gun, whose downstream purpose is to dynamically linearize the desired bunch core. We show that linearization of an appropriately prepared bunch can be achieved via strongly nonlaminar focusing of the sacrificial shock front, while the inner core focuses laminarly. This leads to a natural spatial separation of the two distributions: a dense core surrounded by a diffuse halo of sacrificial charge that can be collimated. Multi-objective genetic algorithm optimizations of the ultra-compact x-ray free electron laser (UCXFEL) injector employ this concept, and we interpret it with an analytic model that agrees well with the simulations. In simulation we demonstrate a final bunch charge of 100 pC, peak current $\sim 30$ A, and a sacrificial charge of 150 pC (250 pC total emitted from cathode) with normalized emittance growth of $<20$ nm-rad due to space charge. This implies a maximum achievable brightness approximately an order of magnitude greater than existing FEL injector designs., Comment: 11 pages, 11 figures, submitted to PRAB

Driven by life-science applications, mega-electron-volt Scanning Transmission Electron Microscope (MeV-STEM) has been proposed to image thick biological samples. The high penetration of inelastic scattering signals of MeV electrons could make the MeV-STEM an appropriate microscope for biological samples as thick as 10 {\mu}m or more with a nanoscale resolution, considering the effect of electron energy, beam broadening and low-dose limit on resolution. The best resolution is inversely related to the sample thickness and changes from 6 nm to 24 nm when the sample thickness increases from 1 {\mu}m to 10 {\mu}m. To achieve such a resolution in STEM, the imaging electrons must be focused on the specimen with a nm size and a mrad semi-convergence angle. This requires an electron beam emittance of a few picometer, which is ~1,000 times smaller than the presently achieved nm emittance, in conjunction with less than 10-4 energy spread and 1 nA current. We numerically simulated two different approaches that are potentially applicable to build a compact MeV-STEM instrument: 1) DC gun, aperture, Superconducting radio frequency (SRF) cavities, and STEM column; 2) SRF gun, aperture, SRF cavities, and STEM column. Beam dynamic simulations show promising results, which meet the needs of an MeV-STEM, a few picometer emittance, less than 10-4 energy spread, and 0.1-1 nA current from both options. Also, we designed a compact STEM column based on permanent quadrupole quintuplet not only to demagnify the beam size from 1 {\mu}m at the source point to 2 nm at the specimen, but also to provide the freedom of changing the magnifications at the specimen and a scanning system to raster the electron beam across the sample with a step size of 2 nm and the repetition rate of 1 MHz. This makes it possible to build a compact MeV-STEM and use it to study thick, large-volume samples in cell biology.

Alkali antimonide semiconductor photocathodes provide a promising platform for the generation of high brightness electron beams, which are necessary for the development of cutting-edge probes including x-ray free electron lasers and ultrafast electron diffraction. However, to harness the intrinsic brightness limits in these compounds, extrinsic degrading factors, including surface roughness and contamination, must be overcome. By exploring the growth of CsxSb thin films monitored by in situ electron diffraction, the conditions to reproducibly synthesize atomically smooth films of CsSb on 3C-SiC (100) and graphene coated TiO2 (110) substrates are identified, and detailed structural, morphological, and electronic characterization is presented. These films combine high quantum efficiency in the visible (up to 1.2% at 400 nm), an easily accessible photoemission threshold of 550 nm, low surface roughness (down to 600 pm on a 1 um scale), and a robustness against oxidation up to 15 times greater then Cs3Sb. These properties suggest that CsSb has the potential to operate as an alternative to Cs$_3$Sb in electron source applications where the demands of the vacuum environment might otherwise preclude the use of traditional alkali antimonides., Comment: 11 pages, 6 figures, 1 table

Ultrafast electron diffraction (UED) is a technique in which short-pulse electron beams can probe the femtosecond-scale evolution of atomic structure in matter driven far from equilibrium. As an accelerator physics challenge, UED imposes stringent constraints on the brightness of the probe electron beam. The low normalized emittance employed in UED, often at the 10 nm scale and below, is particularly sensitive to both applied field aberrations and space charge effects. The role of aberrations is increasingly important in small probe systems that often feature multiple orders of magnitude variations in beam size during transport. In this work, we report the correction of normal quadrupole, skew quadrupole, and sextupole aberrations via dedicated corrector elements in an ultrafast electron micro-diffraction beamline. To do this, we generate precise 4-dimensional phase space maps of rf-compressed electron beams, and find excellent agreement with aberration-free space charge simulations. Finally, we discuss the role a probe-forming aperture can play in improving the brightness of bunches with appreciable space charge effects., Comment: 10 pages, 9 figures, submitted to Physical Review Accelerators and Beams

Ultrafast-optical-pump -- structural-probe measurements, including ultrafast electron and x-ray scattering, provide direct experimental access to the fundamental timescales of atomic motion, and are thus foundational techniques for studying matter out of equilibrium. High-performance detectors are needed in scattering experiments to obtain maximum scientific value from every probe particle. We deploy a hybrid pixel array direct electron detector to perform ultrafast electron diffraction experiments on a WSe$_2$/MoSe$_2$ 2D heterobilayer, resolving the weak features of diffuse scattering and moir\'e superlattice structure without saturating the zero order peak. Enabled by the detector's high frame rate, we show that a chopping technique provides diffraction difference images with signal-to-noise at the shot noise limit. Finally, we demonstrate that a fast detector frame rate coupled with a high repetition rate probe can provide continuous time resolution from femtoseconds to seconds, enabling us to perform a scanning ultrafast electron diffraction experiment that maps thermal transport in WSe$_2$/MoSe$_2$ and resolves distinct diffusion mechanisms in space and time., Comment: Submitted manuscript, 22 pages, 5 figures

Mono- and bi-alkali antimonides, X$_2$YSb (X and Y from Group I), are promising for next-generation electron emitters due to their capability of producing high-quality electron beams. However, these materials are not yet well understood, in part due to the technical challenges in growing pure, ordered alkali antimonides. For example, in the current literature there is a lack of complete understanding of the mechanically stable crystal structures of these materials. As a first step towards understanding this issue, this paper presents an ab initio study of stability of single-crystal mono- and bi-alkali antimonides in the $D0_3$ structure, the structure generally assumed in the literature for these materials. Finding that many of these materials actually are unstable in the $D0_3$ structure, we formulate a new set of Goldschmidt-like tolerance factors that accurately predict $D0_3$ stability using a procedure analogous to machine-learning perceptron-based analysis. Next, we consider possible stable structures for materials that we predict to be unstable in the $D0_3$ structure. Taking as examples the mono- and bi-alkali antimonides Cs$_3$Sb and Cs$_2$KSb, which also are technologically interesting for photoemission and photoabsorption applications, respectively, we note that the most unstable phonon displacements are consistent with the cubic structure, and we therefore perform extensive ab initio searches to identify potential ground-state structures in a cubic lattice. Our X-ray diffraction experiments confirm that indeed these two materials are not stable in the $D0_3$ structure and show scattering that is consistent with our new, proposed stable structures. Finally, we explore ab initio the implications of the breaking of the $D0_3$ symmetry on the electronic structure, showing significant impact on the location of the optical absorption edge., Comment: Submitted to Physical Review Materials

The properties of photoemission electron sources determine the ultimate performance of a wide class of electron accelerators and photon detectors. To date, all high-efficiency visible-light photocathode materials are either polycrystalline or exhibit intrinsic surface disorder, both of which limit emitted electron beam brightness. In this letter we demonstrate the synthesis of epitaxial thin films of Cs$_3$Sb on 3C-SiC (001) using molecular-beam epitaxy. Films as thin as 4 nm have quantum efficiencies exceeding 2\% at 532 nm. We also find that epitaxial films have an order of magnitude larger quantum efficiency at 650 nm than comparable polycrystalline films on Si. Additionally, these films permit angle-resolved photoemission spectroscopy measurements of the electronic structure, which are found to be in good agreement with theory. Epitaxial films open the door to dramatic brightness enhancements via increased efficiency near threshold, reduced surface disorder, and the possibility of engineering new photoemission functionality at the level of single atomic layers., Comment: Submitted Manuscript: 8 pages, 4 figures

We report the design and performance of a time-resolved electron diffraction apparatus capable of producing intense bunches with simultaneously single digit micron probe size, long coherence length, and $200$ fs rms time resolution. We measure the 5d (peak) beam brightness at the sample location in micro-diffraction mode to be $7 \times 10^{13} \ \mathrm{A}/\text{m}^2\text{-rad}^2$. To generate high brightness electron bunches, the system employs high efficiency, low emittance semiconductor photocathodes driven with a wavelength near the photoemission threshold at a repetition rate up to 250 kHz. We characterize spatial, temporal, and reciprocal space resolution of the apparatus. We perform proof-of-principle measurements of ultrafast heating in single crystal Au samples and compare experimental results with simulations that account for the effects of multiple-scattering., Comment: 13 pages, 10 figures, submitted to Structural Dynamics

In an effort to increase spatial and temporal resolution of ultrafast electron diffraction and microscopy, ultra-high brightness photocathodes are actively sought to improve electron beam quality. Beam dynamics codes often approximate the Coulomb interaction with mean-field space charge, which is a good approximation in traditional beams. However, point-to-point Coulomb effects, such as disorder induced heating and the Boersch effect, can not be neglected in cold, dense beams produced by such photocathodes. In this paper, we introduce two new numerical methods to calculate the important effects of the photocathode image charge when using a point-to-point interaction model. Equipped with an accurate model of the image charge, we calculate the effects of point-to-point interactions on two high brightness photoemission beamlines for ultrafast diffraction. The first beamline uses a 200 keV gun, whereas the second uses a 5 MeV gun, each operating in the single-shot diffraction regime with $10^5$ electrons/pulse. Assuming a zero photoemission temperature, it is shown that including stochastic Coulomb effects increases the final emittance of these beamlines by over a factor of 2 and decreases the peak transverse phase space density by over a factor of 3 as compared to mean-field simulations. We then introduce a method to compute the energy released by disorder induced heating using the pair correlation function. This disorder induced heating energy was found to scale very near the theoretical result for stationary ultracold plasmas, and it accounts for over half of the emittance growth above mean-field simulations., Comment: 15 pages, 17 figures, submitted to PRAB

In preparation for a demonstration of optical stochastic cooling in the Cornell Electron Storage Ring (CESR) we have developed a particle tracking simulation to study the relevant beam dynamics. Optical radiation emitted in the pickup undulator gives a momentum kick to that same particle in the kicker undulator. The optics of the electron bypass from pickup to kicker couples betatron amplitude and momentum offset to path length so that the momentum kick reduces emittance and momentum spread. Nearby electrons contribute an incoherent noise. Layout of the bypass line is presented that accommodates optics with a range of transverse and longitudinal cooling parameters. The simulation is used to determine cooling rates and their dependence on bunch and lattice parameters for bypass optics with distinct emittance and momentum acceptance.

A proposed experiment to demonstrate Optical Stochastic Cooling (OSC) in the Cornell Electron Storage Ring (CESR) based on an arc-bypass design is presented. This arc-bypass provides significantly longer optical delay than the dog-leg style chicane, opening up the possibility of a multi-pass or staged optical amplifier that can achieve the gains required for effective cooling of hadron or heavy-ions. Beyond introducing the arc-bypass, in this paper we study the stability requirements for the dipoles comprising it and investigate the use of an optical feedback system to relax the dipole and light-path stability tolerances.

In the field of beam physics, two frontier topics have taken center stage due to their potential to enable new approaches to discovery in a wide swath of science. These areas are: advanced, high gradient acceleration techniques, and x-ray free electron lasers (XFELs). Further, there is intense interest in the marriage of these two fields, with the goal of producing a very compact XFEL. In this context, recent advances in high gradient radio-frequency cryogenic copper structure research have opened the door to the use of surface electric fields between 250 and 500 MV/m. Such an approach is foreseen to enable a new generation of photoinjectors with six-dimensional beam brightness beyond the current state-of-the-art by well over an order of magnitude. This advance is an essential ingredient enabling an ultra-compact XFEL (UC-XFEL). In addition, one may accelerate these bright beams to GeV scale in less than 10 meters. Such an injector, when combined with inverse free electron laser-based bunching techniques can produce multi-kA beams with unprecedented beam quality, quantified by ~50 nm-rad normalized emittances. These beams, when injected into innovative, short-period (1-10 mm) undulators uniquely enable UC-XFELs having footprints consistent with university-scale laboratories. We describe the architecture and predicted performance of this novel light source, which promises photon production per pulse of a few percent of existing XFEL sources. We review implementation issues including collective beam effects, compact x-ray optics systems, and other relevant technical challenges. To illustrate the potential of such a light source to fundamentally change the current paradigm of XFELs with their limited access, we examine possible applications in biology, chemistry, materials, atomic physics, industry, and medicine which may profit from this new model of performing XFEL science., Comment: 80 pages, 24 figures

In this article, we report on the development of a time-of-flight based electron energy analyzer capable of measuring the 3-D momentum and energy distributions of very low energy (meV-scale) photoemitted electrons. This analyzer is capable of measuring energy and 3-D momentum distributions of electrons with energies down to 1 meV with a sub-meV energy resolution. This analyzer is an ideal tool for studying photoemission processes very close to the photoemission threshold and also for studying the physics of photoemission based electron sources.

Using an 800 nm, 45 fs pulse-front-tilted laser we demonstrate a record 315 keV energy gain in a dual grating dielectric laser accelerator (DLA) and average accelerating gradients of 560 MV/m over 0.5 mm. These results open a new regime in DLA characterized by significant evolution of the beam distribution in the longitudinal phase space, corresponding to >1/4 of a synchrotron oscillation. By tilting the laser wavefront we control the resonant velocity of the DLA and observe a net energy gain, indicating that a tapered optical phase could be used to achieve very high energy gain., Comment: 5 pages, 5 figures

Recent investigations of RF copper structures operated at cryogenic temperatures performed by a SLAC-UCLA collaboration have shown a dramatic increase in the maximum surface electric field, to 500 MV/m. We examine use of these fields to enable very high field cryogenic photoinjectors that can attain over an order of magnitude increase in peak electron beam brightness. We present beam dynamics studies relevant to X-ray FEL injectors, using start-to-end simulations that show the high brightness and low emittance of this source enables operation of a compact FEL reaching a photon energy of 80 keV. The preservation of beam brightness in compression, exploiting micro-bunching techniques is discussed. While the gain in brightness at high field is due to increase of the emission current density, further increases in brightness due to lowering of the intrinsic cathode emittance in cryogenic operation are also enabled. While the original proposal for this type of cryogenic, ultra-high field photoinjector has emphasized S-band designs, there are numerous potential advantages that may be conferred by operation in C-band. We examine issues related to experimental implementation in C-band, and expected performance of this type of device in a future hard X-ray FEL such as MaRIE., Comment: 10 pages, 5 figures, to appear in Proceedings of 2018 European Advanced Accelerator Conference, Nuclear Instruments and Methods

We present a methodology for designing and measuring pulse front tilt in an ultrafast laser for use in dielectric laser acceleration. Previous research into dielectric laser accelerating modules has focused on measuring high accelerating gradients in novel structures, but has done so only for short electron-laser coupling lengths. Here we demonstrate an optical design to extend the laser-electron interaction to 1mm., Comment: 5 pages, 4 figures, Submitted to NIMA for proceedings of EAAC 2017

Laser powered dielectric structures achieve high-gradient particle acceleration by taking advantage of modern laser technology capable of producing electric fields in excess of 10GV/m. These fields can drive the bulk dielectric beyond its linear response, and break the phase synchronicity between the accelerating field and the electrons. We show how control of the pulse dispersion can be used to compensate the effect of self-phase modulation and maximize the energy gain in the laser accelerator.In our experiment, a high brightness 8MeV e-beam is used to probe accelerating fields of 1.8GV/m in a 'grating-reset' dielectric structure illuminated by a 45fs laser pulse with a fluence of 0.7J/cm$^2$., Comment: 7 pages, 5 figures

The heating of the electronic distribution of a copper photocathode due to an intense drive laser pulse is calculated under the two-temperature model using fluences and pulse lengths typical in RF photoinjector operation. Using the finite temperature-extended relations for the photocathode intrinsic emittance and quantum efficiency, the time-dependent emittance growth due to the same photoemission laser pulse is calculated. This laser heating is seen to limit the intrinsic emittance achievable for photoinjectors using short laser pulses and low quantum efficiency metal photocathodes. A pump-probe photocathode experiment in a standard 1.6 cell S-band gun is proposed, in which simulations show the time dependent thermal emittance modulation within the bunch from laser heating can persist for meters downstream and, in principle, be measured using a slice emittance diagnostic.

We present the results of multi-objective genetic algorithm optimizations of a potential single shot ultra fast electron diffraction beamline utilizing a 100 MV/m 1.6 cell normal conducting rf (NCRF) gun, as well as a 9 cell 2pi/3 bunching cavity placed between two solenoids. Optimizations of the transverse projected emittance as a function of bunch charge are presented and discussed in terms of the scaling laws derived in the charge saturation limit. Additionally, optimization of the transverse coherence length as a function of final rms bunch length at the sample location have been performed for a charge of 1e6 electrons. Analysis of the solutions is discussed, as are the effects of disorder induced heating. In particular, for a charge of $10^6$ electrons and final beam size greater than or equal to 25 microns, we found a relative coherence length of 0.07, 0.1, and 0.2 nm/micron for a final bunch length of approximately 5, 30, and 100 fs, respectively. These results demonstrate the viability of using genetic algorithms in the design and operation of ultrafast electron diffraction beamlines., Comment: arXiv admin note: substantial text overlap with arXiv:1510.07738

We present the results of an experiment where a short focal length (~ 1.3 cm) permanent magnet electron lens is used to image micron-size features of a metal sample in a single shot, using an ultra- high brightness ps-long 4 MeV electron beam from a radiofrequency photoinjector. Magnifcation ratios in excess of 30x were obtained using a triplet of compact, small gap (3.5 mm), Halbach-style permanent magnet quadrupoles with nearly 600 T/m field gradients. These results pave the way to- wards single shot time-resolved electron microscopy and open new opportunities in the applications of high brightness electron beams., Comment: 5 pages, 6 figures

Recent studies of the performance of radio-frequency (RF) copper cavities operated at cryogenic temperatures have shown a dramatic increase in the maximum achievable surface electric field. We propose to exploit this development to enable a new generation of photoinjectors operated at cryogenic temperatures that may attain, through enhancement of the launch field at the photocathode, a significant increase in five-dimensional electron beam brightness. We present detailed studies of the beam dynamics associated with such a system, by examining an S-band photoinjector operated at 250 MV/m peak electric field that reaches normalized emittances in the 40 nm-rad range at charges (100-200 pC) suitable for use in a hard X-ray free-electron laser (XFEL) scenario based on the LCLS. In this case, we show by start-to-end simulations that the properties of this source may give rise to high efficiency operation of an XFEL, and permit extension of the photon energy reach by an order of magnitude, to over 80 keV. The brightness needed for such XFELs is achieved through low source emittances in tandem with high current after compression. In the XFEL examples analyzed, the emittances during final compression are preserved using micro-bunching techniques. Extreme low emittance scenarios obtained at pC charge, appropriate for significantly extending temporal resolution limits of ultrafast electron diffraction and microscopy experiments, are also reviewed. While the increase in brightness in a cryogenic photoinjector is mainly due to the augmentation of the emission current density via field enhancement, further possible increases in performance arising from lowering the intrinsic cathode emittance in cryogenic operation are also analyzed. Issues in experimental implementation, including cavity optimization for lowering cryogenic thermal dissipation, external coupling, and cryo-cooler system are discussed., Comment: 34 pages, 17 figures, 127 references. submitted to Physical Review Accelerators and Beams