Synchronized beamline at FLASH2 based on high-order harmonic generation for two-color dynamics studies.

We present the design, integration, and operation of the novel vacuum ultraviolet (VUV) beamline installed at the free-electron laser (FEL) FLASH. The VUV source is based on high-order harmonic generation (HHG) in gas and is driven by an optical laser system synchronized with the timing structure of the FEL. Ultrashort pulses in the spectral range from 10 to 40 eV are coupled with the FEL in the beamline FL26, which features a reaction microscope (REMI) permanent endstation for time-resolved studies of ultrafast dynamics in atomic and molecular targets. The connection of the high-pressure gas HHG source to the ultra-high vacuum FEL beamline requires a compact and reliable system, able to encounter the challenging vacuum requirements and coupling conditions. First commissioning results show the successful operation of the beamline, reaching a VUV focused beam size of about 20 µm at the REMI endstation. Proof-of-principle photo-electron momentum measurements in argon indicate the source capabilities for future two-color pump-probe experiments.

A nozzle for high-density supersonic gas jets at elevated temperatures.

We present the development of a gas nozzle providing high-density gas at elevated temperatures inside a vacuum environment. Fused silica is used as the nozzle material to allow the placement of the nozzle tip in close proximity to an intense, high-power laser beam, while minimizing the risk of sputtering nozzle tip material into the vacuum chamber. Elevating the gas temperature increases the gas-jet forward velocity, allowing us to replenish the gas volume in the laser-gas interaction region between consecutive laser shots. The nozzle accommodates a 50 µm opening hole from which a supersonic gas jet emerges. Heater wires are used to bring the nozzle temperature up to 730 °C, while a cooling unit ensures that the nozzle mount and the glued nozzle-to-mount connection is kept at a temperature below 50 °C. The presented nozzle design is used for high-order harmonic generation in hot gases using gas backing pressures of up to 124 bars.

Sub-cycle ionization dynamics revealed by trajectory resolved, elliptically-driven high-order harmonic generation.

The sub-cycle dynamics of electrons driven by strong laser fields is central to the emerging field of attosecond science. We demonstrate how the dynamics can be probed through high-order harmonic generation, where different trajectories leading to the same harmonic order are initiated at different times, thereby probing different field strengths. We find large differences between the trajectories with respect to both their sensitivity to driving field ellipticity and resonant enhancement. To accurately describe the ellipticity dependence of the long trajectory harmonics we must include a sub-cycle change of the initial velocity distribution of the electron and its excursion time. The resonant enhancement is observed only for the long trajectory contribution of a particular harmonic when a window resonance in argon, which is off-resonant in the field-free case, is shifted into resonance due to a large dynamic Stark shift.

Attosecond pulse walk-off in high-order harmonic generation.

We study the influence of the generation conditions on the group delay of attosecond pulses in high-order harmonic generation in gases. The group delay relative to the fundamental field is found to decrease with increasing gas pressure in the generation cell, reflecting a temporal walk-off due to the dispersive properties of the nonlinear medium. This effect is well reproduced using an on-axis phase-matching model of high-order harmonic generation in an absorbing gas.

Macroscopic effects in noncollinear high-order harmonic generation.

We study two-color high-order harmonic generation using an intense driving field and its weak second harmonic, crossed under a small angle in the focus. Employing sum- and difference-frequency generation processes, such a noncollinear scheme can be used to measure and control macroscopic phase matching effects by utilizing a geometrical phase mismatch component, which depends on the noncollinear angle. We further show how spatial phase effects in the generation volume are mapped out into the far field allowing a direct analogy with temporal carrier envelope effects in attosecond pulse generation.

High-order harmonic generation using a high-repetition-rate turnkey laser.

We generate high-order harmonics at high pulse repetition rates using a turnkey laser. High-order harmonics at 400 kHz are observed when argon is used as target gas. In neon, we achieve generation of photons with energies exceeding 90 eV (∼13 nm) at 20 kHz. We measure a photon flux of up to 4.4 × 10(10) photons per second per harmonic in argon at 100 kHz. Many experiments employing high-order harmonics would benefit from higher repetition rates, and the user-friendly operation opens up for applications of coherent extreme ultra-violet pulses in new research areas.

A high-flux high-order harmonic source.

We develop and implement an experimental strategy for the generation of high-energy high-order harmonics (HHG) in gases for studies of nonlinear processes in the soft x-ray region. We generate high-order harmonics by focusing a high energy Ti:Sapphire laser into a gas cell filled with argon or neon. The energy per pulse is optimized by an automated control of the multiple parameters that influence the generation process. This optimization procedure allows us to obtain energies per pulse and harmonic order as high as 200 nJ in argon and 20 nJ in neon, with good spatial properties, using a loose focusing geometry (f#≈400) and a 20 mm long medium. We also theoretically examine the macroscopic conditions for absorption-limited conversion efficiency and optimization of the HHG pulse energy for high-energy laser systems.

Efficient high-order harmonic generation boosted by below-threshold harmonics.

High-order harmonic generation (HHG) in gases has been established as an important technique for the generation of coherent extreme ultraviolet (XUV) pulses at ultrashort time scales. Its main drawback, however, is the low conversion efficiency, setting limits for many applications, such as ultrafast coherent imaging, nonlinear processes in the XUV range, or seeded free electron lasers. Here we introduce a novel scheme based on using below-threshold harmonics, generated in a "seeding cell", to boost the HHG process in a "generation cell", placed further downstream in the focused laser beam. By modifying the fundamental driving field, these low-order harmonics alter the ionization step of the nonlinear HHG process. Our dual-cell scheme enhances the conversion efficiency of HHG, opening the path for the realization of robust intense attosecond XUV sources.

Digital in-line holography on amplitude and phase objects prepared with electron beam lithography.

We report on the fabrication and characterization of amplitude and phase samples consisting of well defined Au or Al features formed on ultrathin silicon nitride membranes. The samples were manufactured using electron beam lithography, metallization and a lift-off technique, which allow precise lateral control and thickness of the metal features. The fabricated specimens were evaluated by conventional microscopy, atomic force microscopy and with the digital in-line holography set-up at the Lund Laser Centre. The latter uses high-order harmonic generation as a light source, and is capable of recovering both the shape and phase shifting properties of the samples. We report on the details of the sample production and on the imaging tests with the holography set-up.

Spectrally resolved maker fringes in high-order harmonic generation.

We investigate macroscopic interference effects in high-order harmonic generation using a Ti:sapphire laser operating at a 100 kHz repetition rate. The structure and behavior of spectral and spatial interference fringes are explained and analytically described by transient phase matching of the long electron trajectory contribution. Time-frequency mapping due to the temporal chirp of the harmonic emission allows us to observe Maker fringes directly in the spectral domain.