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.

Supercontinuum generation in OHQ-N2S organic crystal driven by intense terahertz fields.

A laser supercontinuum is generated by cross-phase modulation (XPM) driven by an intense terahertz (THz) field in organic crystal OHQ-N2S. In this highly nonlinear medium, the THz electric field induces a time-varying optical phase modulation, which causes a spectacular spectral broadening and shifting of a co-propagating near-infrared laser pulse. The effect is enabled by the large electro-optic coefficient, the low absorption, and the good velocity matching between the laser and the THz pulse over the OHQ-N2S crystal thickness. The XPM occurs when the THz field is aligned along the polar axis of the OHQ-N2S. The results display a promising pathway for ultrafast control of the spectral and temporal properties of laser pulses using THz stimuli.

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.

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.

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.

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.

A universal route to efficient non-linear response via Thomson scattering in linear solids.

Non-linear materials are cornerstones of modern optics and electronics. Strong dependence on the intrinsic properties of particular materials, however, inhibits the at-will extension of demanding non-linear effects, especially those second-order ones, to widely adopted centrosymmetric materials (for example, silicon) and technologically important burgeoning spectral domains (for example, terahertz frequencies). Here we introduce a universal route to efficient non-linear responses enabled by exciting non-linear Thomson scattering, a fundamental process in electrodynamics that was known to occur only in relativistic electrons in metamaterial composed of linear materials. Such a mechanism modulates the trajectory of charges, either intrinsically or extrinsically provided in solids, at twice the driving frequency, allowing second-harmonic generation at terahertz frequencies on crystalline silicon with extremely large non-linear susceptibility in our proof-of-concept experiments. By offering a substantially material- and frequency-independent platform, our approach opens new possibilities in the fields of on-demand non-linear optics, terahertz sources, strong field light-solid interactions and integrated photonic circuits.

An X-ray free-electron laser with a highly configurable undulator and integrated chicanes for tailored pulse properties.

X-ray free-electron lasers (FELs) are state-of-the-art scientific tools capable to study matter on the scale of atomic processes. Since the initial operation of X-ray FELs more than a decade ago, several facilities with upgraded performance have been put in operation. Here we present the first lasing results of Athos, the soft X-ray FEL beamline of SwissFEL at the Paul Scherrer Institute in Switzerland. Athos features an undulator layout based on short APPLE-X modules providing full polarisation control, interleaved with small magnetic chicanes. This versatile configuration allows for many operational modes, giving control over many FEL properties. We show, for example, a 35% reduction of the required undulator length to achieve FEL saturation with respect to standard undulator configurations. We also demonstrate the generation of more powerful pulses than the ones obtained in typical undulators. Athos represents a fundamental step forward in the design of FEL facilities, creating opportunities in FEL-based sciences.

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.

Can energetic terahertz pulses initiate surface catalytic reactions on the picosecond time scale?

In preparation for picosecond pump-probe experiments at the SwissFEL X-ray laser facility, the feasibility of collectively initiating surface chemical reactions using energetic pulses of terahertz radiation is being tested.

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.