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.

In multi electron beam systems, "Neighbours Matter".

In the Multi beam source (MBS) of our Multi Beam Scanning Electron Microscope (MBSEM), an aperture lens array (ALA) splits the emission cone of the Schottky field emitter into multiple beamlets. When the apertures in the ALA are close to each other, the ALA can introduce aberrations to these beamlets through the electrostatic interaction of neighbouring apertures with each aperture's lens field. When the apertures are arranged in a square grid pattern, the aberration causes fourfold astigmatism. The effect on the beam spot is analyzed through a combination of 3D simulations and experimental validation. To counterbalance the fourfold astigmatism, a correction scheme is proposed in which a slightly non-round profile is applied to the aperture lenses.

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.

Pulse length, energy spread, and temporal evolution of electron pulses generated with an ultrafast beam blanker.

Crucial for the field of ultrafast electron microscopy is the creation of sub-picosecond, high brightness electron pulses. The use of a blanker to chop the beam that originates from a high brightness Schottky source may provide an attractive alternative to direct pulsed laser illumination of the source. We have recently presented the concept of a laser-triggered ultrafast beam blanker and argued that generation of 100 fs pulses could be possible [Weppelman et al., Ultramicroscopy 184, 8-17 (2017)]. However, a detailed analysis of the influence of a deflection field changing sign on sub-picoseconds time scale on the quality of the resulting electron pulses has so far been lacking. Here, we present such an analysis using time-dependent, three-dimensional numerical simulations to evaluate the time-evolution of deflection fields in and around a micrometers-scale deflector connected to a photo-conductive switch. Further particle tracing through the time-dependent fields allows us to evaluate beam quality parameters such as energy spread and temporal broadening. We show that with a shielded, "tunnel-type" design of the beam blanker limiting the spatial extent of fringe fields outside the blanker, the blanker-induced energy spread can be limited to 0.5 eV. Moreover, our results confirm that it could be possible to bring laser-triggered 100 fs focused electron pulses on the sample using a miniaturized ultrafast beam blanker. This would enable us to resolve ultrafast dynamics using focused electron pulses in an SEM or STEM.

Complementary cathodoluminescence lifetime imaging configurations in a scanning electron microscope.

Cathodoluminescence (CL) spectroscopy provides a powerful way to characterize optical properties of materials with deep-subwavelength spatial resolution. While CL imaging to obtain optical spectra is a well-developed technology, imaging CL lifetimes with nanoscale resolution has only been explored in a few studies. In this paper we compare three different time-resolved CL techniques and compare their characteristics. Two configurations are based on the acquisition of CL decay traces using a pulsed electron beam that is generated either with an ultra-fast beam blanker, which is placed in the electron column, or by photoemission from a laser-driven electron cathode. The third configuration uses measurements of the autocorrelation function g(2) of the CL signal using either a continuous or a pulsed electron beam. The three techniques are compared in terms of complexity of implementation, spatial and temporal resolution, and measurement accuracy as a function of electron dose. A single sample of InGaN/GaN quantum wells is investigated to enable a direct comparison of lifetime measurement characteristics of the three techniques. The g(2)-based method provides decay measurements at the best spatial resolution, as it leaves the electron column configuration unaffected. The pulsed-beam methods provide better detail on the temporal excitation and decay dynamics. The ultra-fast blanker configuration delivers electron pulses as short as 30 ps at 5 keV and 250 ps at 30 keV. The repetition rate can be chosen arbitrarily up to 80 MHz and requires a conjugate plane geometry in the electron column that reduces the spatial resolution in our microscope. The photoemission configuration, pumped with 250 fs 257 nm pulses at a repetition rate from 10 kHz to 25 MHz, allows creation of electron pulses down to a few ps, with some loss in spatial resolution.

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.

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.

Subnanosecond Thomson scattering on a vacuum arc discharge in tin vapor.

In a previous series of Thomson scattering (TS) experiments on an extreme ultraviolet producing vacuum arc discharge in tin vapor, background radiation emitted by the plasma was found to make measurements impossible for all parts of the discharge except the prepinch phase. To reduce the level of recorded background radiation, we have built a setup for time and space resolved subnanosecond TS. Results obtained with this new setup are presented for experiments on previously inaccessible parts of the discharge--the ignition phase, pinch phase, and decay phase. For the first two, measurements have been performed at different heights in the plasma. Electron densities for the pinch phase have been derived. For the decay phase, the electron densities confirm previous Stark broadening data. From the overall results, a more complete picture of the plasma evolution can be formed.

Comparison of experimental and simulated extreme ultraviolet spectra of xenon and tin discharges.

Xenon and tin both are working elements applied in discharge plasmas that are being developed for application in extreme ultraviolet (EUV) lithography. Their spectra in the 10-21-nm-wavelength range have been analyzed. A fully analytical collisional-radiative model, including departure from equilibrium due to a net ionization rate, was used to simulate the EUV spectra. Detailed Hartree-Fock calculations, using the COWAN package, were applied for determination of the energy levels and optical transition probabilities of the 8+ to 12+ ions of both elements. For the calculation of the radiation, the opacity of the plasma was taken into account. Time-resolved measurements of the spectra from ionizing phases of two different discharge plasmas were corrected for the wavelength-dependent sensitivity of the spectrometer, and compared to the results of the simulations. Fairly good agreement between the experiments and the model calculations has been found.

Characterization of a vacuum-arc discharge in tin vapor using time-resolved plasma imaging and extreme ultraviolet spectrometry.

Discharge sources in tin vapor have recently been receiving increased attention as candidate extreme ultraviolet (EUV) light sources for application in semiconductor lithography, because of their favorable spectrum near 13.5 nm. In the ASML EUV laboratory, time-resolved pinhole imaging in the EUV and two-dimensional imaging in visible light have been applied for qualitative characterization of the evolution of a vacuum-arc tin vapor discharge. An EUV spectrometer has been used to find the dominant ionization stages of tin as a function of time during the plasma evolution of the discharge.

Collective Thomson scattering experiments on a tin vapor discharge in the prepinch phase.

Partially collective Thomson scattering measurements have been performed on a triggered vacuum arc in tin vapor, which is a candidate source of extreme ultraviolet light for application in semiconductor lithography. In this paper, results on the electron densities and temperatures are presented for the prepinch phase of the discharge. Electron densities and temperatures increase from 1 x 10(23) m(-3) to 1 x 10(24) m(-3) and from 5 eV to over 30 eV, respectively, in about 100 ns. The results are confirmed by Stark broadening data.

Stark broadening experiments on a vacuum arc discharge in tin vapor.

Pinched discharge plasmas in tin vapor are candidates for application in future semiconductor lithography tools. This paper presents time-resolved measurements of Stark broadened linewidths in a pulsed tin discharge. Stark broadening parameters have been determined for four lines of the Sn III spectrum in the range from 522 to 538 nm, based on a cross-calibration to a Sn II line with a previously known Stark width. The influence of the electron temperature on the Stark widths is discussed. Results for the electron densities in the discharge are presented and compared to Thomson scattering results.

Time-resolved pinhole camera imaging and extreme ultraviolet spectrometry on a hollow cathode discharge in xenon.

A pinhole camera, an extreme ultraviolet (EUV) spectrometer, a fast gatable multichannel plate EUV detector, and a digital camera have been installed on the ASML EUV laboratory setup to perform time-resolved pinhole imaging and EUV spectroscopy on a copy of the Philips EUV hollow cathode discharge plasma source. The main properties of the setup have been characterized. Time-resolved measurements within the plasma pulse in the EUV have been performed on this source. Specific features of the plasma, such as a ring shape in the initiation phase and a propagating sphere during the pinch phase, have either been discovered or confirmed experimentally. Relative populations of various ionization stages in the pinch plasma have been estimated on the basis of line intensities and calculated transition probabilities. The changes in relative line intensities of a single ionization stage can be explained by a combination of temperature and excitation/deexcitation balance effects. Experiments with argon dilution on a newer version of the source show considerable effect on the shape of the xenon EUV spectrum.