Non-thermal structural transformation of diamond driven by x-rays.

Intense x-ray pulses can cause the non-thermal structural transformation of diamond. At the SACLA XFEL facility, pump x-ray pulses triggered this phase transition, and probe x-ray pulses produced diffraction patterns. Time delays were observed from 0 to 250 fs, and the x-ray dose varied from 0.9 to 8.0 eV/atom. The intensity of the (111), (220), and (311) diffraction peaks decreased with time, indicating a disordering of the crystal lattice. From a Debye-Waller analysis, the rms atomic displacements perpendicular to the (111) planes were observed to be significantly larger than those perpendicular to the (220) or (311) planes. At a long time delay of 33 ms, graphite (002) diffraction indicates that graphitization did occur above a threshold dose of 1.2 eV/atom. These experimental results are in qualitative agreement with XTANT+ simulations using a hybrid model based on density-functional tight-binding molecular dynamics.

Effect of Auger recombination on transient optical properties in XUV and soft X-ray irradiated silicon nitride.

Spatially encoded measurements of transient optical transmissivity became a standard tool for temporal diagnostics of free-electron-laser (FEL) pulses, as well as for the arrival time measurements in X-ray pump and optical probe experiments. The modern experimental techniques can measure changes in optical coefficients with a temporal resolution better than 10 fs. This, in an ideal case, would imply a similar resolution for the temporal pulse properties and the arrival time jitter between the FEL and optical laser pulses. However, carrier transport within the material and out of its surface, as well as carrier recombination may, in addition, significantly decrease the number of carriers. This would strongly affect the transient optical properties, making the diagnostic measurement inaccurate. Below we analyze in detail the effects of those processes on the optical properties of XUV and soft X-ray irradiated Si[Formula: see text]N[Formula: see text], on sub-picosecond timescales. Si[Formula: see text]N[Formula: see text] is a wide-gap insulating material widely used for FEL pulse diagnostics. Theoretical predictions are compared with the published results of two experiments at FERMI and LCLS facilities, and with our own recent measurement. The comparison indicates that three body Auger recombination strongly affects the optical response of Si[Formula: see text]N[Formula: see text] after its collisional ionization stops. By deconvolving the contribution of Auger recombination, in future applications one could regain a high temporal resolution for the reconstruction of the FEL pulse properties measured with a Si[Formula: see text]N[Formula: see text]-based diagnostics tool.

High-sensitivity x-ray/optical cross-correlator for next generation free-electron lasers.

We design and realize an arrival time diagnostic for ultrashort X-ray pulses achieving unprecedented high sensitivity in the soft X-ray regime via cross-correlation with a ≈1550 nm optical laser. An interferometric detection scheme is combined with a multi-layer sample design to greatly improve the sensitivity of the measurement. We achieve up to 275% of relative signal change when exposed to 1.6 mJ/cm2 of soft X-rays at 530 eV, more than a hundred-fold improvement in sensitivity as compared to previously reported techniques. The resolution of the arrival time measurement is estimated to around 2.8 fs (rms). The demonstrated X-ray arrival time monitor paves the way for sub-10 fs-level timing jitter at high repetition rate X-ray facilities.

Enabling high repetition rate nonlinear THz science with a kilowatt-class sub-100 fs laser source.

Manipulating the atomic and electronic structure of matter with strong terahertz (THz) fields while probing the response with ultrafast pulses at x-ray free electron lasers (FELs) has offered unique insights into a multitude of physical phenomena in solid state and atomic physics. Recent upgrades of x-ray FEL facilities are pushing to much higher repetition rates, enabling unprecedented signal-to-noise ratio for pump probe experiments. This requires the development of suitable THz pump sources that are able to deliver intense pulses at compatible repetition rates. Here we present a high-power laser-driven THz source based on optical rectification in LiNbO3 using tilted pulse front pumping. Our source is driven by a kilowatt-level Yb:YAG amplifier system operating at 100 kHz repetition rate and employing nonlinear spectral broadening and recompression to achieve sub-100 fs pulses with pulse energies up to 7 mJ that are necessary for high THz conversion efficiency and peak field strength. We demonstrate a maximum of 144 mW average THz power (1.44 µJ pulse energy), consisting of single-cycle pulses centered at 0.6 THz with a peak electric field strength exceeding 150 kV/cm. These high field pulses open up a range of possibilities for nonlinear time-resolved THz experiments at unprecedented rates.

100 W high-repetition-rate near-infrared optical parametric chirped pulse amplifier.

New high-repetition-rate x-ray free electron lasers (XFELs) require for their operation highly reliable ultrafast laser systems with high pulse energy, high repetition rate, and high average power. In this Letter, we present high-average-power scaling of near-infrared optical parametric chirped pulse amplification (OPCPA) in potassium titanyl arsenate (KTA) with tunable center wavelengths from 1.5 to 2.0 µm. Using a three-stage amplification scheme and a kW-level InnoSlab Yb:YAG pump amplifier for the final non-collinear KTA stage, we demonstrate an amplified output power of 106.2 W at a center wavelength of 1.75 µm and 100 kHz. Idler absorption introduces a potential upper limit on the average power scaling of center wavelengths <1.70 µm. Future scaling of average power to hundreds of Watts is possible at center wavelengths ≥1.70 µm.

Photon diagnostics at the FLASH THz beamline.

The THz beamline at FLASH, DESY, provides both tunable (1-300 THz) narrow-bandwidth (∼10%) and broad-bandwidth intense (up to 150 uJ) THz pulses delivered in 1 MHz bursts and naturally synchronized with free-electron laser X-ray pulses. Combination of these pulses, along with the auxiliary NIR and VIS ultrashort lasers, supports a plethora of dynamic investigations in physics, material science and biology. The unique features of the FLASH THz pulses and the accelerator source, however, bring along a set of challenges in the diagnostics of their key parameters: pulse energy, spectral, temporal and spatial profiles. Here, these challenges are discussed and the pulse diagnostic tools developed at FLASH are presented. In particular, a radiometric power measurement is presented that enables the derivation of the average pulse energy within a pulse burst across the spectral range, jitter-corrected electro-optical sampling for the full spectro-temporal pulse characterization, spatial beam profiling along the beam transport line and at the sample, and a lamellar grating based Fourier transform infrared spectrometer for the on-line assessment of the average THz pulse spectra. Corresponding measurement results provide a comprehensive insight into the THz beamline capabilities.

High average power 88 W OPCPA system for high-repetition-rate experiments at the LCLS x-ray free-electron laser.

We present a 100 kHz, sub-20 fs optical parametric chirped-pulse amplifier (OPCPA) system delivering 88.6 W average power at a center wavelength of 800 nm. The seed pulses are derived from the pump laser via white-light continuum generation and are amplified in three non-collinear OPCPA stages. The final two high-power stages are pumped with a 661 W Yb:YAG InnoSlab amplifier. A simple and robust design is used for the OPCPA system to avoid thermal effects and enhance long-term stability, resulting in excellent beam quality and high conversion efficiency. To the best of our knowledge, this is the highest average power OPCPA system reported to date.

The phase-contrast imaging instrument at the matter in extreme conditions endstation at LCLS.

We describe the phase-contrast imaging instrument at the Matter in Extreme Conditions (MEC) endstation of the Linac Coherent Light Source. The instrument can image phenomena with a spatial resolution of a few hundreds of nanometers and at the same time reveal the atomic structure through X-ray diffraction, with a temporal resolution better than 100 fs. It was specifically designed for studies relevant to high-energy-density science and can monitor, e.g., shock fronts, phase transitions, or void collapses. This versatile instrument was commissioned last year and is now available to the MEC user community.

Optical laser systems at the Linac Coherent Light Source.

Ultrafast optical lasers play an essential role in exploiting the unique capabilities of recently commissioned X-ray free-electron laser facilities such as the Linac Coherent Light Source (LCLS). Pump-probe experimental techniques reveal ultrafast dynamics in atomic and molecular processes and reveal new insights in chemistry, biology, material science and high-energy-density physics. This manuscript describes the laser systems and experimental methods that enable cutting-edge optical laser/X-ray pump-probe experiments to be performed at LCLS.

Investigation of two-beam-pumped noncollinear optical parametric chirped-pulse amplification for the generation of few-cycle light pulses.

We demonstrate a new and compact Phi-plane-pumped noncollinear optical parametric chirped-pulse amplification (NOPCPA) scheme for broadband pulse amplification, which is based on two-beam-pumping (TBP) at 532 nm. We employ type-I phase-matching in a 5 mm long BBO crystal with moderate pump intensities to preserve the temporal pulse contrast. Amplification and compression of the signal pulse from 675 nm - 970 nm is demonstrated, which results in the generation of 7.1-fs light pulses containing 0.35 mJ energy. In this context, we investigate the pump-to-signal energy conversion efficiency for TBP-NOPCPA and outline details for few-cycle pulse characterization. Furthermore, it is verified, that the interference at the intersection of the two pump beams does not degrade the signal beam spatial profile. It is theoretically shown that the accumulated OPA phase partially compensates for wave-vector mismatch and leads to extended broadband amplification. The experimental outcome is supported by numerical split-step simulations of the parametric signal gain, including pump depletion and parametric fluorescence.

Generation of sub-three-cycle, 16 TW light pulses by using noncollinear optical parametric chirped-pulse amplification.

We present a two-stage noncollinear optical parametric chirped-pulse amplification system that generates 7.9 fs pulses containing 130 mJ of energy at an 805 nm central wavelength and 10 Hz repetition rate. These 16 TW light pulses are compressed to within 5% of their Fourier limit and are carefully characterized by the use of home-built pulse diagnostics. The contrast ratio before the main pulse has been measured as 10(-4), 10(-8), and 10(-11) at t=-3.3 ps, t=-5 ps, and t=-30 ps, respectively. This source allows for experiments in a regime of relativistic light-matter interactions and attosecond science.

Dispersion management for a sub-10-fs, 10 TW optical parametric chirped-pulse amplifier.

We report the amplification of three-cycle, 8.5 fs optical pulses in a near-infrared noncollinear optical parametric chirped-pulse amplifier (OPCPA) up to energies of 80 mJ. Improved dispersion management in the amplifier by means of a combination of reflection grisms and a chirped-mirror stretcher allowed us to recompress the amplified pulses to within 6% of their Fourier limit. The novel ultrabroad, ultraprecise dispersion control technology presented in this work opens the way to scaling multiterawatt technology to even shorter pulses by optimizing the OPCPA bandwidth.

90 mJ parametric chirped pulse amplification of 10 fs pulses.

We demonstrate the amplification of broadband pulses from a Ti:Sapphire oscillator by non-collinear optical parametric chirped-pulse amplification technique in a type-I BBO crystal to energies of 90 mJ. Partial compression of the amplified pulses is demonstrated down to a 10 fs duration. These parameters come in combination with good spatial quality and focusability of the amplified beam.