Arrival time fluctuation of the SwissFEL photocathode laser: characterization by a single color balanced cross correlator.

The arrival time jitter and drift of the photocathode drive laser has an important impact on the performance of a Free-Electron-Laser (FEL). It adversely affects the beam energy jitter, bunch length jitter and bunch arrival time jitter, which becomes especially important for pump-probe experiments with femtosecond time resolution. To measure both parameters background free and stabilize the drift of the Yb:CaF2 based laser we use a well designed balanced optical cross correlator. In this paper we present our results using this device and focus particularly on the performance of the amplifier. We achieve a laser drift of less than 200 fs during 60 h, a 4.5 fs rms jitter of the amplifier relative to its seeding oscillator and 11 fs rms for the whole laser relative to a reference clock integrated from 2 mHz to 100 Hz.

SwissFEL Aramis beamline photon diagnostics. Erratum.

The list of authors in the paper by Juranic et al. (2018) [J. Synchrotron Rad. 25, 1238-1248] is corrected.

SwissFEL Aramis beamline photon diagnostics.

The SwissFEL Aramis beamline, covering the photon energies between 1.77 keV and 12.7 keV, features a suite of online photon diagnostics tools to help both users and FEL operators in analysing data and optimizing experimental and beamline performance. Scientists will be able to obtain information about the flux, spectrum, position, pulse length, and arrival time jitter versus the experimental laser for every photon pulse, with further information about beam shape and size available through the use of destructive screens. This manuscript is an overview of the diagnostics tools available at SwissFEL and presents their design, working principles and capabilities. It also features new developments like the first implementation of a THz-streaking based temporal diagnostics for a hard X-ray FEL, capable of measuring pulse lengths to 5 fs r.m.s. or better.

Deformable mirror for wavefront shaping of infrared radiation.

We present proof-of-principle results on terahertz wavefront shaping by means of a deformable mirror (DM). The DM is based on a reflective gold-coated steel membrane pushed by 35 powerful stepper actuators to enable a surface deformation of up to 1 mm out of equilibrium. The maximum excursion is equivalent to 10 wavelengths of the terahertz source centered at 3 THz and, thus, offers excellent opportunities for shaping the terahertz wavefront and beam intensity profile. As a proof of principle, we demonstrate terahertz focal spot optimization towards the diffraction limit, focal depth shifting, and terahertz imaging application. The large aperture DM offers new opportunities for the wavefront manipulation demanded by high-field terahertz science. The extreme excursion range of the DM will be beneficial for beam shaping at other wavelengths, such as visible and UV.

Single-silicon CCD-CMOS platform for multi-spectral detection from terahertz to x-rays.

Charge-coupled devices (CCDs) are a well-established imaging technology in the visible and x-ray frequency ranges. However, the small quantum photon energies of terahertz radiation have hindered the use of this mature semiconductor technological platform in this frequency range, leaving terahertz imaging totally dependent on low-resolution bolometer technologies. Recently, it has been shown that silicon CCDs can detect terahertz photons at a high field, but the detection sensitivity is limited. Here we show that silicon, complementary metal-oxide-semiconductor (CMOS) technology offers enhanced detection sensitivity of almost two orders of magnitude, compared to CCDs. Our findings allow us to extend the low-frequency terahertz cutoff to less than 2 THz, nearly closing the technological gap with electronic imagers operating up to 1 THz. Furthermore, with the silicon CCD/CMOS technology being sensitive to mid-infrared (mid-IR) and the x-ray ranges, we introduce silicon as a single detector platform from 1 EHz to 2 THz. This overcomes the present challenge in spatially overlapping a terahertz/mid-IR pump and x-ray probe radiation at facilities such as free electron lasers, synchrotron, and laser-based x-ray sources.

Opportunities for Chemistry at the SwissFEL X-ray Free Electron Laser.

X-ray techniques have long been applied to chemical research, ranging from powder diffraction tools to analyse material structure to X-ray fluorescence measurements for sample composition. The development of high-brightness, accelerator-based X-ray sources has allowed chemists to use similar techniques but on more demanding samples and using more photon-hungry methods. X-ray Free Electron Lasers (XFELs) are the latest in the development of these large-scale user facilities, opening up new avenues of research and the possibility of more advanced applications for a range of research. The SwissFEL XFEL project at the Paul Scherrer Institute will begin user operation in the hard X-ray (2.1-12.4 keV) photon energy range in 2018 with soft X-ray (240-1930 eV) user operation to follow and here we will present the details of this project, it's operating capabilities, and some aspects of the experimental stations that will be particularly attractive for chemistry research. SwissFEL is a revolutionary new machine that will complement and extend the time-resolved chemistry efforts in the Swiss research community.

Subcycle Extreme Nonlinearities in GaP Induced by an Ultrastrong Terahertz Field.

We report on the experimental observation of extreme laser spectral broadening and a change in optical transmission in gallium phosphite induced by 25 MV/cm terahertz (THz) single-cycle internal field. Such intense THz radiation leads to twofold transient modifications of the optical properties in the electro-optical crystal. First, the electric field provokes extensive cross-phase modulation via the χ^{(2)} and χ^{(3)} nonlinearities on a copropagating 50 fs near infrared laser pulse which turns into 500% spectral broadening. Second, we observe an instantaneous change of the optical transmission occurring at the THz field which is alleged to interband Zener tunneling and charge carrier density modification by impact ionization turning the semiconductor in a metal-like transient state. The presented scheme displays a pathway to coherently control the optical properties of semiconductors on an ultrafast time scale by a strong THz field.

THz streak camera method for synchronous arrival time measurement of two-color hard X-ray FEL pulses.

The two-color operation of free electron laser (FEL) facilities allows the delivery of two FEL pulses with different energies, which opens new possibilities for user experiments. Measuring the arrival time of both FEL pulses relative to the external experimental laser and to each other improves the temporal resolution of the experiments using the two-color FEL beam and helps to monitor the performance of the machine itself. This work reports on the first simultaneous measurement of the arrival times of two hard X-ray FEL pulses with the THz streak camera. Measuring the arrival time of the two FEL pulses, the relative delay between them was calculated and compared to the set values. Furthermore, we present the first comparison of the THz streak camera method to the method of FEL induced transient transmission. The results indicate a good agreement between the two methods.

High-power femtosecond Raman frequency shifter.

We report on the generation of broadband, high-energy femtosecond pulses centered at 1.28 µm by stimulated Raman scattering in a pressurized hydrogen cell. Stimulated Raman scattering is performed by two chirped and delayed pulses originating from a multi-mJ Ti:sapphire amplifier. The Stokes pulse carries record-high energy of 4.4 mJ and is recompressed down to 66 fs by a reflective grating pair. We characterized the short-wavelength mid-infrared source in view of energy stability, beam profile, and conversion efficiency at repetition rates of 100 and 10 Hz. The demonstrated high-energy frequency shifter will benefit intense THz sources based on highly nonlinear organic crystals.

Intense THz source based on BNA organic crystal pumped at Ti:sapphire wavelength.

We report on high-energy terahertz pulses by optical rectification (OR) in the organic crystal N-benzyl-2-methyl-4-nitroaniline (BNA) directly pumped by a conventional Ti:sapphire amplifier. The simple scheme provides an optical-to-terahertz conversion efficiency of 0.25% when pumped by collimated laser pulses with a duration of 50 fs and a central wavelength of 800 nm. The generated radiation spans frequencies between 0.2 and 3 THz. We measured the damage threshold, as well as the dependency of the conversion efficiency on the pump fluence, pump wavelength, and pulse duration.

Comparison of Thermal Detector Arrays for Off-Axis THz Holography and Real-Time THz Imaging.

In terahertz (THz) materials science, imaging by scanning prevails when low power THz sources are used. However, the application of array detectors operating with high power THz sources is increasingly reported. We compare the imaging properties of four different array detectors that are able to record THz radiation directly. Two micro-bolometer arrays are designed for infrared imaging in the 8-14 µm wavelength range, but are based on different absorber materials (i) vanadium oxide; (ii) amorphous silicon; (iii) a micro-bolometer array optimized for recording THz radiation based on silicon nitride; and (iv) a pyroelectric array detector for THz beam profile measurements. THz wavelengths of 96.5 µm, 118.8 µm, and 393.6 µm from a powerful far infrared laser were used to assess the technical performance in terms of signal to noise ratio, detector response and detectivity. The usefulness of the detectors for beam profiling and digital holography is assessed. Finally, the potential and limitation for real-time digital holography are discussed.

Femtosecond resolution timing jitter correction on a TW scale Ti:sapphire laser system for FEL pump-probe experiments.

Intense ultrashort pulse lasers are used for fs resolution pump-probe experiments more and more at large scale facilities, such as free electron lasers (FEL). Measurement of the arrival time of the laser pulses and stabilization to the machine or other sub-systems on the target, is crucial for high time-resolution measurements. In this work we report on a single shot, spectrally resolved, non-collinear cross-correlator with sub-fs resolution. With a feedback applied we keep the output of the TW class Ti:sapphire amplifier chain in time with the seed oscillator to ~3 fs RMS level for several hours. This is well below the typical pulse duration used at FELs and supports fs resolution pump-probe experiments. Short term jitter and long term timing drift measurements are presented. Applicability to other wavelengths and integration into the timing infrastructure of the FEL are also covered to show the full potential of the device.

High-performing nonlinear visualization of terahertz radiation on a silicon charge-coupled device.

Photoinduced electron transitions can lead to significant changes of the macroscopic electronic properties in semiconductors. This principle is responsible for the detection of light with charge-coupled devices. Their spectral sensitivity is limited by the semiconductor bandgap which has restricted their visualization capabilities to the optical, ultraviolet, and X-ray regimes. The absence of an imaging device in the low frequency terahertz range has severely hampered the advance of terahertz imaging applications in the past. Here we introduce a high-performing imaging concept to the terahertz range. On the basis of a silicon charge-coupled device we visualize 5-13 THz radiation with photon energy under 2% of the sensor's band-gap energy. The unprecedented small pitch and large number of pixels allow the visualization of complex terahertz radiation patterns in real time and with high spatial detail. This advance will have a great impact on a wide range of terahertz imaging disciplines.

Spectrally intense terahertz source based on triangular Selenium.

The intensity of a nonlinear terahertz (THz) source is primarily given by its spectral density. In this letter, we introduce triangular Selinium (Se) as a novel THz emitter and show numerically its superior properties to the currently used crystals for intense THz generation. The excellent phase matching enables the applicability of elongated Se crystals which results in very high spectral flatness and broad THz bandwidth (0.5-3.5 THz), high conversion efficiency and THz pulse energy.The spectral THz density produced by optical rectification in Selenium exceeds those from contemporary crystal-based THz sources.

Demonstration of a low-frequency three-dimensional terahertz bullet with extreme brightness.

The brightness of a light source defines its applicability to nonlinear phenomena in science. Bright low-frequency terahertz (<5 THz) radiation confined to a diffraction-limited spot size is a present hurdle because of the broad bandwidth and long wavelengths associated with terahertz (THz) pulses and because of the lack of THz wavefront correctors. Here using a present-technology system, we employ a wavefront manipulation concept with focusing optimization leading to spatio-temporal confinement of THz energy at its physical limits to the least possible three-dimensional light bullet volume of wavelength-cubic. Our scheme relies on finding the optimum settings of pump wavefront curvature and post generation beam divergence. This leads to a regime of extremely bright PW m(-2) level THz radiation with peak fields up to 8.3 GV m(-1) and 27.7 T surpassing by far any other system. The presented results are foreseen to have a great impact on nonlinear THz applications in different science disciplines.

Tailoring single-cycle electromagnetic pulses in the 2-9 THz frequency range using DAST/SiO2 multilayer structures pumped at Ti:sapphire wavelength.

We present a numerical parametric study of single-cycle electromagnetic pulse generation in a DAST/SiO2multilayer structure via collinear optical rectification of 800 nm femtosecond laser pulses. It is shown that modifications of the thicknesses of the DAST and SiO2layers allow tuning of the average frequency of the generated THz pulses in the frequency range from 3 to 6 THz. The laser-to-THz energy conversion efficiency in the proposed structures is compared with that in a bulk DAST crystal and a quasi-phase-matching periodically poled DAST crystal and shows significant enhancement.

Spatiotemporal focusing dynamics of intense supercontinuum THz pulses.

High-field terahertz (THz) single-cycle pulses with 1.5 MV/cm are generated by optical rectification in the stilbazolium salt crystal 4-N,N-dimethylamino-4'-N'-methyl-stilbazolium 2,4,6-trimethylbenzenesulfonate. We show experimentally that the generated THz transient carrying 5 octaves (0.15 to 5.5 THz) undergoes a complex time-frequency evolution when tightly focused, and we present a model based on three independent oscillating dipoles capable to describe this anomalous field evolution. Finally, we present a method to control the absolute phase of such supercontinuum THz pulses as an essential tool for future field-sensitive investigations.

Scaling submillimeter single-cycle transients toward megavolts per centimeter field strength via optical rectification in the organic crystal OH1.

We present the generation of high-power single-cycle terahertz (THz) pulses in the organic salt crystal 2-[3-(4-hydroxystyryl)-5.5-dimethylcyclohex-2-enylidene]malononitrile or OH1. Broadband THz radiation with a central frequency of 1.5 THz (λ(c)=200 µm) and high electric field strength of 440 kV/cm is produced by optical rectification driven by the signal of a powerful femtosecond optical parametric amplifier. A 1.5% pump to THz energy conversion efficiency is reported, and pulse energy stability better than 1% RMS is achieved. An approach toward the realization of higher field strength is discussed.

Ultrabroadband TW-class Ti:sapphire laser system with adjustable central wavelength, bandwidth and multi-color operation.

We demonstrate a versatile tunable and highly stable ultrabroadband Ti:sapphire chirped pulse amplification system with a compressed pulse energy of 20 mJ at 100 Hz repetition rate. High power Ti:Sa systems in principle do not offer wavelength tunability due to gain narrowing. Here we demonstrate transform limited pulse generation from 15 fs to 94 fs with tunable central wavelength (λc from 755 nm to 845 nm) and bandwidth (130 nm<Δλ<16 nm) as well as multi-color, time synchronized, sub-100 fs pulses with user defined central wavelength separation. The unique wavelength tunability capabilities have been expanded into the UV and deep-UV by second and third harmonic generation with excellent energy stability. Enhanced energy stability is achieved by multiplexing six ultrastable diode-based solid state pump lasers.

Towards high-power single-cycle THz laser for initiating high-field-sensitive phenomena.

Powerful THz radiation confined in one field period or less is an adequate tool for triggering nonlinear actions. We show results towards the realization of a tunable high-power THz source based on a laser-driven frequency conversion scheme in plasma and nonlinear crystals. A powerful THz source in combination with the future X-ray Free Electron Laser facility in Switzerland (SwissFEL) holds promise for exciting experiments in a variety of different research areas.