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.

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.

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.

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.

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.

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.

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.

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.

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.

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.

Analytical model of an isolated single-atom electron source.

An analytical model of a single-atom electron source is presented, where electrons are created by near-threshold photoionization of an isolated atom. The model considers the classical dynamics of the electron just after the photon absorption, i.e. its motion in the potential of a singly charged ion and a uniform electric field used for acceleration. From closed expressions for the asymptotic transverse electron velocities and trajectories, the effective source temperature and the virtual source size can be calculated. The influence of the acceleration field strength and the ionization laser energy on these properties has been studied. With this model, a single-atom electron source with the optimum electron beam properties can be designed. Furthermore, we show that the model is also applicable to ionization of rubidium atoms, and thus also describes the ultracold electron source, which is based on photoionization of laser-cooled alkali atoms.

A proposal for fs-electron microscopy experiments on high-energy excitations in solids.

Recent advances in ultrafast technology enable both the study and the control of materials properties thanks to the ability to record high temporal resolution movies of their transformations, or the ability to generate new states of matter by selecting ad hoc an excitation to drive the system out of equilibrium. The holy grail of this type of experiments is to combine a high tuneability of the excitation with a wide observation window. For example, this is achieved in multidimensional optical spectroscopy where the response to several excitation energies is monitored in a broad energy range by a large bandwidth optical pulse. In this article, the possibility to combine the chemical sensitivity of intense tuneable X-rays pulses from a free electron laser, with the wide range of observables available in an ultrafast transmission electron microscope is discussed. The requirements for such experiments are quantified via estimates based on state of the art experiments and simulations, and it is proposed that ultrafast electron imaging, diffraction and spectroscopy experiments can be performed in combination with a chemically selective X-ray excitation of materials.

Ultrafast electron diffraction using an ultracold source.

The study of structural dynamics of complex macromolecular crystals using electrons requires bunches of sufficient coherence and charge. We present diffraction patterns from graphite, obtained with bunches from an ultracold electron source, based on femtosecond near-threshold photoionization of a laser-cooled atomic gas. By varying the photoionization wavelength, we change the effective source temperature from 300 K to 10 K, resulting in a concomitant change in the width of the diffraction peaks, which is consistent with independently measured source parameters. This constitutes a direct measurement of the beam coherence of this ultracold source and confirms its suitability for protein crystal diffraction.

Effective temperature of an ultracold electron source based on near-threshold photoionization.

We present a detailed description of measurements of the effective temperature of a pulsed electron source, based on near-threshold photoionization of laser-cooled atoms. The temperature is determined by electron beam waist scans, source size measurements with ion beams, and analysis with an accurate beam line model. Experimental data is presented for the source temperature as a function of the wavelength of the photoionization laser, for both nanosecond and femtosecond ionization pulses. For the nanosecond laser, temperatures as low as 14 ± 3 K were found; for femtosecond photoionization, 30 ± 5 K is possible. With a typical source size of 25 µm, this results in electron bunches with a relative transverse coherence length in the 10⁻4 range and an emittance of a few nm rad.