Direct Observation of Sub-Poissonian Temporal Statistics in a Continuous Free-Electron Beam with Subpicosecond Resolution.

We present a novel method to measure the arrival time statistics of continuous electron beams with subpicosecond resolution, based on the combination of an rf deflection cavity and fast single electron imaging. We observe Poissonian statistics within time bins from 100 to 2 ns and increasingly pronounced sub-Poissonian statistics as the time bin decreases from 2 ps to 340 fs. This 2D streak camera, in principle, enables femtosecond-level arrival time measurements, paving the way to observing Pauli blocking effects in electron beams and thus serving as an essential diagnostic tool toward degenerate electron beam sources for free-electron quantum optics.

Subpicosecond Ultracold Electron Source.

We present the first observation of subpicosecond electron bunches from an ultracold electron source. This source is based on near-threshold, two-step, femtosecond photoionization of laser-cooled rubidium gas in a grating magneto-optical trap. Bunch lengths as short as 735±7 fs (rms) have been measured in the self-compression point of the source by means of ponderomotive scattering of the electrons by a 25 fs, 800 nm laser pulse. The observed temporal structure of the electron bunch depends on the central wavelength of the ionization laser pulse, in agreement with detailed simulations of the atomic photoionization process. This shows that the bunch length limit imposed by the atomic photoionization process has been reached.

RF acceleration of ultracold electron bunches.

The ultrafast and ultracold electron source, based on laser cooling and trapping of atomic gas and its subsequent near-threshold two-step photoionization, is capable of generating electron bunches with a high transverse brightness at energies of roughly 10 keV. This paper investigates the possibility of increasing the range of applications of this source by accelerating the bunch using radio frequency electromagnetic fields. Bunch energies up to 35 keV are measured by analyzing the diffraction patterns generated from a mono-crystalline gold sample. It is found that the normalized transverse emittance is largely preserved during acceleration.

Photodiode-based time zero determination for ultrafast electron microscopy.

Pump-probe experiments in ultrafast electron microscopy require temporal overlap between the pump and probe pulses. Accurate measurements of the time delay between them allows for the determination of the time zero, the moment in time where both pulses perfectly overlap. In this work, we present the use of a photodiode-based alignment method for these time zero measurements. The cheap and easy-to-use device consists of a photodiode in a sample holder and enables us to temporally align individual, single-electron pulses with femtosecond laser pulses. In a first device, a temporal resolution of 24 ps is obtained, limited by the photodiode design. Future work will utilize a smaller photodiode with a lower capacitance, which will increase the temporal resolution and add spatial resolution as well. This upgrade will bring the method toward the micrometer and picosecond spatiotemporal resolution.

Isolated attosecond X-ray pulses from superradiant thomson scattering by a relativistic chirped electron mirror.

Time-resolved investigation of electron dynamics relies on the generation of isolated attosecond pulses in the (soft) X-ray regime. Thomson scattering is a source of high energy radiation of increasing prevalence in modern labs, complementing large scale facilities like undulators and X-ray free electron lasers. We propose a scheme to generate isolated attosecond X-ray pulses based on Thomson scattering by colliding microbunched electrons on a chirped laser pulse. The electrons collectively act as a relativistic chirped mirror, which superradiantly reflects the laser pulse into a single localized beat. As such, this technique extends chirped pulse compression, developed for radar and applied in optics, to the X-ray regime. In this paper we theoretically show that, by using this approach, attosecond soft X-ray pulses with GW peak power can be generated from pC electron bunches at tens of MeV electron beam energy. While we propose the generation of few cycle X-ray pulses on a table-top system, the theory is universally scalable over the electromagnetic spectrum.

Design and characterization of a resonant microwave cavity as a diagnostic for ultracold plasmas.

We present the design and commissioning of a resonant microwave cavity as a novel diagnostic for the study of ultracold plasmas. This diagnostic is based on the measurements of the shift in the resonance frequency of the cavity, induced by an ultracold plasma that is created from a laser-cooled gas inside. This method is simultaneously non-destructive, very fast (nanosecond temporal resolution), highly sensitive, and applicable to all ultracold plasmas. To create an ultracold plasma, we implement a compact magneto-optical trap based on a diffraction grating chip inside a 5 GHz resonant microwave cavity. We are able to laser cool and trap (7.25 ± 0.03) × 107 rubidium atoms inside the cavity, which are turned into an ultracold plasma by two-step pulsed (nanosecond or femtosecond) photo-ionization. We present a detailed characterization of the cavity, and we demonstrate how it can be used as a fast and sensitive probe to monitor the evolution of ultracold plasmas non-destructively. The temporal resolution of the diagnostic is determined by measuring the delayed frequency shift following femtosecond photo-ionization. We find a response time of 18 ± 2 ns, which agrees well with the value determined from the cavity quality factor and resonance frequency.

Phase-space manipulation of ultracold ion bunches with time-dependent fields.

All applications of high brightness ion beams depend on the possibility to precisely manipulate the trajectories of the ions or, more generally, to control their phase-space distribution. We show that the combination of a laser-cooled ion source and time-dependent acceleration fields gives new possibilities to perform precise phase-space control. We demonstrate reduction of the longitudinal energy spread and realization of a lens with control over its focal length and sign, as well as the sign of the spherical aberrations. This creates new possibilities to correct for the spherical and chromatic aberrations which are presently limiting the spatial resolution.

Compression of subrelativistic space-charge-dominated electron bunches for single-shot femtosecond electron diffraction.

We demonstrate the compression of 95 keV, space-charge-dominated electron bunches to sub-100 fs durations. These bunches have sufficient charge (200 fC) and are of sufficient quality to capture a diffraction pattern with a single shot, which we demonstrate by a diffraction experiment on a polycrystalline gold foil. Compression is realized by means of velocity bunching by inverting the positive space-charge-induced velocity chirp. This inversion is induced by the oscillatory longitudinal electric field of a 3 GHz radio-frequency cavity. The arrival time jitter is measured to be 80 fs.

Magnetic field-enhanced beam monitor for ionizing radiation.

For the microwave cavity resonance spectroscopy based non-destructive beam monitor for ionizing radiation, an addition-which adapts the approach to conditions where only little ionization takes place due to, e.g., small ionization cross sections, low gas pressures, and low photon fluxes-is presented and demonstrated. In this experiment, a magnetic field with a strength of 57 ± 1 mT was used to extend the lifetime of the afterglow of an extreme ultraviolet-induced plasma by a factor of ∼5. Magnetic trapping is expected to be most successful in preventing the decay of ephemeral free electrons created by low-energy photons. Good agreement has been found between the experimental results and the decay rates calculated based on the ambipolar and classical collision diffusion models.

Ultracold electron source for single-shot, ultrafast electron diffraction.

Ultrafast electron diffraction (UED) enables studies of structural dynamics at atomic length and timescales, i.e., 0.1 nm and 0.1 ps, in single-shot mode. At present UED experiments are based on femtosecond laser photoemission from solid state cathodes. These photoemission sources perform excellently, but are not sufficiently bright for single-shot studies of, for example, biomolecular samples. We propose a new type of electron source, based on near-threshold photoionization of a laser-cooled and trapped atomic gas. The electron temperature of these sources can be as low as 10 K, implying an increase in brightness by orders of magnitude. We investigate a setup consisting of an ultracold electron source and standard radio-frequency acceleration techniques by GPT tracking simulations. The simulations use realistic fields and include all pairwise Coulomb interactions. We show that in this setup 120 keV, 0.1 pC electron bunches can be produced with a longitudinal emittance sufficiently small for enabling sub-100 fs bunch lengths at 1% relative energy spread. A transverse root-mean-square normalized emittance of epsilon(x) = 10 nm is obtained, significantly better than from photoemission sources. Correlations in transverse phase-space indicate that the transverse emittance can be improved even further, enabling single-shot studies of biomolecular samples.

Design and characterization of dielectric filled TM110 microwave cavities for ultrafast electron microscopy.

Microwave cavities oscillating in the TM110 mode can be used as dynamic electron-optical elements inside an electron microscope. By filling the cavity with a dielectric material, it becomes more compact and power efficient, facilitating the implementation in an electron microscope. However, the incorporation of the dielectric material makes the manufacturing process more difficult. Presented here are the steps taken to characterize the dielectric material and to reproducibly fabricate dielectric filled cavities. Also presented are two versions with improved capabilities. The first, called a dual-mode cavity, is designed to support two modes simultaneously. The second has been optimized for low power consumption. With this optimized cavity, a magnetic field strength of 2.84 ± 0.07 mT was generated at an input power of 14.2 ± 0.2 W. Due to the low input powers and small dimensions, these dielectric cavities are ideal as electron-optical elements for electron microscopy setups.

High quality ultrafast transmission electron microscopy using resonant microwave cavities.

Ultrashort, low-emittance electron pulses can be created at a high repetition rate by using a TM110 deflection cavity to sweep a continuous beam across an aperture. These pulses can be used for time-resolved electron microscopy with atomic spatial and temporal resolution at relatively large average currents. In order to demonstrate this, a cavity has been inserted in a transmission electron microscope, and picosecond pulses have been created. No significant increase of either emittance or energy spread has been measured for these pulses. At a peak current of 814 ±â€¯2 pA, the root-mean-square transverse normalized emittance of the electron pulses is ɛn,x=(2.7±0.1)·10-12 m rad in the direction parallel to the streak of the cavity, and ɛn,y=(2.5±0.1)·10-12 m rad in the perpendicular direction for pulses with a pulse length of 1.1-1.3 ps. Under the same conditions, the emittance of the continuous beam is ɛn,x=ɛn,y=(2.5±0.1)·10-12 m rad. Furthermore, for both the pulsed and the continuous beam a full width at half maximum energy spread of 0.95 ±â€¯0.05 eV has been measured.

Time-of-flight electron energy loss spectroscopy by longitudinal phase space manipulation with microwave cavities.

The possibility to perform high-resolution time-resolved electron energy loss spectroscopy has the potential to impact a broad range of research fields. Resolving small energy losses with ultrashort electron pulses, however, is an enormous challenge due to the low average brightness of a pulsed beam. In this paper, we propose to use time-of-flight measurements combined with longitudinal phase space manipulation using resonant microwave cavities. This allows for both an accurate detection of energy losses with a high current throughput and efficient monochromation. First, a proof-of-principle experiment is presented, showing that with the incorporation of a compression cavity the flight time resolution can be improved significantly. Then, it is shown through simulations that by adding a cavity-based monochromation technique, a full-width-at-half-maximum energy resolution of 22 meV can be achieved with 3.1 ps pulses at a beam energy of 30 keV with currently available technology. By combining state-of-the-art energy resolutions with a pulsed electron beam, the technique proposed here opens up the way to detecting short-lived excitations within the regime of highly collective physics.

Theory and particle tracking simulations of a resonant radiofrequency deflection cavity in TM110 mode for ultrafast electron microscopy.

We present a theoretical description of resonant radiofrequency (RF) deflecting cavities in TM110 mode as dynamic optical elements for ultrafast electron microscopy. We first derive the optical transfer matrix of an ideal pillbox cavity and use a Courant-Snyder formalism to calculate the 6D phase space propagation of a Gaussian electron distribution through the cavity. We derive closed, analytic expressions for the increase in transverse emittance and energy spread of the electron distribution. We demonstrate that for the special case of a beam focused in the center of the cavity, the low emittance and low energy spread of a high quality beam can be maintained, which allows high-repetition rate, ultrafast electron microscopy with 100 fs temporal resolution combined with the atomic resolution of a high-end TEM. This is confirmed by charged particle tracking simulations using a realistic cavity geometry, including fringe fields at the cavity entrance and exit apertures.

Improving temporal resolution of ultrafast electron diffraction by eliminating arrival time jitter induced by radiofrequency bunch compression cavities.

The temporal resolution of sub-relativistic ultrafast electron diffraction (UED) is generally limited by the radio frequency (RF) phase and amplitude jitter of the RF lenses that are used to compress the electron pulses. We theoretically show how to circumvent this limitation by using a combination of several RF compression cavities. We show that if powered by the same RF source and with a proper choice of RF field strengths, RF phases, and distances between the cavities, the combined arrival time jitter due to RF phase jitter of the cavities is cancelled at the compression point. We also show that the effect of RF amplitude jitter on the temporal resolution is negligible when passing through the cavity at a RF phase optimal for (de)compression. This will allow improvement of the temporal resolution in UED experiments to well below 100 fs.

Pulse length of ultracold electron bunches extracted from a laser cooled gas.

We present measurements of the pulse length of ultracold electron bunches generated by near-threshold two-photon photoionization of a laser-cooled gas. The pulse length has been measured using a resonant 3 GHz deflecting cavity in TM110 mode. We have measured the pulse length in three ionization regimes. The first is direct two-photon photoionization using only a 480 nm femtosecond laser pulse, which results in short (∼15 ps) but hot (∼104 K) electron bunches. The second regime is just-above-threshold femtosecond photoionization employing the combination of a continuous-wave 780 nm excitation laser and a tunable 480 nm femtosecond ionization laser which results in both ultracold (∼10 K) and ultrafast (∼25 ps) electron bunches. These pulses typically contain ∼103 electrons and have a root-mean-square normalized transverse beam emittance of 1.5 ± 0.1 nm rad. The measured pulse lengths are limited by the energy spread associated with the longitudinal size of the ionization volume, as expected. The third regime is just-below-threshold ionization which produces Rydberg states which slowly ionize on microsecond time scales.

Single-cycle surface plasmon polaritons on a bare metal wire excited by relativistic electrons.

Terahertz (THz) pulses are applied in areas as diverse as materials science, communication and biosensing. Techniques for subwavelength concentration of THz pulses give access to a rapidly growing range of spatial scales and field intensities. Here we experimentally demonstrate a method to generate intense THz pulses on a metal wire, thereby introducing the possibility of wave-guiding and focussing of the full THz pulse energy to subwavelength spotsizes. This enables endoscopic sensing, single-shot subwavelength THz imaging and study of strongly nonlinear THz phenomena. We generate THz surface plasmon polaritons (SPPs) by launching electron bunches onto the tip of a bare metal wire. Bunches with 160 pC charge and ≈6 ps duration yield SPPs with 6-10 ps duration and 0.4±0.1 MV m-1 electric field strength on a 1.5 mm diameter aluminium wire. These are the most intense SPPs reported on a wire. The SPPs are shown to propagate around a 90° bend.

Time-of-flight electron energy loss spectroscopy using TM110 deflection cavities.

We demonstrate the use of two TM110 resonant cavities to generate ultrashort electron pulses and subsequently measure electron energy losses in a time-of-flight type of setup. The method utilizes two synchronized microwave cavities separated by a drift space of 1.45 m. The setup has an energy resolution of 12 ± 2 eV FWHM at 30 keV, with an upper limit for the temporal resolution of 2.7 ± 0.4 ps. Both the time and energy resolution are currently limited by the brightness of the tungsten filament electron gun used. Through simulations, it is shown that an energy resolution of 0.95 eV and a temporal resolution of 110 fs can be achieved using an electron gun with a higher brightness. With this, a new method is provided for time-resolved electron spectroscopy without the need for elaborate laser setups or expensive magnetic spectrometers.

Suspended crystalline films of protein hydrophobin I (HFBI).

Protein interfaces play an essential role in both natural and man-made materials as stabilizers, sensors, catalysts, and selective channels for ions and small molecules. Probing the molecular arrangement within such interfaces is of prime importance to understand the relation between structure and functionality. Here we report on the preparation and characterization of large area suspended crystalline films of class II hydrophobin HFBI. This small, amphiphilic globular protein readily self-assembles at the air-water interface into a 2D hexagonal lattice which can be transferred onto a holey carbon electron microscopy grid yielding large areas of hundreds of square micrometers intact hydrophobin film spun across micron-sized holes. Fourier transform analysis of low-dose electron microscopy images and selected area electron diffraction profiles reveal a unit cell dimension a=5.6±0.1nm, in agreement with reported atomic force microscopy studies on solid substrates and grazing incidence X-ray scattering experiments at the air-water interface. These findings constitute the first step towards the utilization of large-area suspended crystalline hydrophobin films as membranes for ultrapurification and chiral separation or as biological substrates for ultrafast electron diffraction.

Nonlinear electrostatic emittance compensation in kA, fs electron bunches.

Nonlinear space-charge effects play an important role in emittance growth in the production of kA electron bunches with a bunch length much smaller than the bunch diameter. We propose a scheme employing the radial third-order component of an electrostatic acceleration field, to fully compensate the nonlinear space-charge effects. This results in minimal transverse root-mean-square emittance. The principle is demonstrated using our design simulations of a device for the production of high-quality, high-current, subpicosecond electron bunches using electrostatic acceleration in a 1 GV/m field. Simulations using the GPT code produce a bunch of 100 pC and 73 fs full width at half maximum pulse width, resulting in a peak current of about 1.2 kA at an energy of 2 MeV. The compensation scheme reduces the root-mean-square emittance by 34% to 0.4pi mm mrad.