Linnea Rading

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.

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.

Gating attosecond pulses in a noncollinear geometry

The efficient generation of isolated attosecond pulses (IAPs), giving access to ultrafast electron dynamics in various systems, is a key challenge in attosecond science. IAPs can be produced by confining the extreme ultraviolet emission generated by an intense laser pulse to a single field half-cycle or, as shown recently, by employing angular streaking methods. Here, we experimentally demonstrate the angular streaking of attosecond pulse trains in a noncollinear geometry, leading to the emission of angularly separated IAPs. The noncollinear geometry simplifies the separation of the fundamental laser field and the generated pulses, making this scheme promising for intracavity attosecond pulse generation, thus opening new possibilities for high-repetition-rate attosecond sources.

Two-photon double ionization of neon using an intense attosecond pulse train

We present a demonstration of two-photon double ionization of neon using an intense extreme ultraviolet (XUV) attosecond pulse train (APT) in a photon energy regime where both direct and sequential mechanisms are allowed. For an APT generated through high-order harmonic generation (HHG) in argon we achieve a total pulse energy close to 1μJ, a central energy of 35 eV, and a total bandwidth of ∼30 eV. The APT is focused by broadband optics in a neon gas target to an intensity of 3×1012Wcm−2. By tuning the photon energy across the threshold for the sequential process the double ionization signal can be turned on and off, indicating that the two-photon double ionization predominantly occurs through a sequential process. The demonstrated performance opens up possibilities for future XUV-XUV pump-probe experiments with attosecond temporal resolution in a photon energy range where it is possible to unravel the dynamics behind direct versus sequential double ionization and the associated electron correlation effects.

Anisotropic photoemission time delays close to a Fano resonance

Electron correlation and multielectron effects are fundamental interactions that govern many physical and chemical processes in atomic, molecular and solid state systems. The process of autoionization, induced by resonant excitation of electrons into discrete states present in the spectral continuum of atomic and molecular targets, is mediated by electron correlation. Here we investigate the attosecond photoemission dynamics in argon in the 20–40 eV spectral range, in the vicinity of the 3s−1np autoionizing resonances. We present measurements of the differential photoionization cross section and extract energy and angle-dependent atomic time delays with an attosecond interferometric method. With the support of a theoretical model, we are able to attribute a large part of the measured time delay anisotropy to the presence of autoionizing resonances, which not only distort the phase of the emitted photoelectron wave packet but also introduce an angular dependence.Ionization time delays are of interest in understanding the photoionization mechanism in atoms and molecules in ultra-short time scales. Here the authors investigate the angular dependence of photoionization time delays in the presence of an autoionizing resonance in argon atom using RABBITT technique.

Interference in the angular distribution of photoelectrons in superimposed XUV and optical laser fields

The angular distribution of photoelectrons ejected during the ionization of Ne atoms by extreme ultraviolet (XUV) free-electron laser radiation in the presence of an intense near infrared (NIR) dressing field was investigated experimentally and theoretically. A highly nonlinear process with absorption and emission of more than ten NIR photons results in the formation of numerous sidebands. The amplitude of the sidebands varies strongly with the emission angle and the angular distribution pattern reveals clear signatures of interferences between the different angular momenta for the outgoing electron in the multi-photon process. As a specific feature, the central photoelectron line is characterized at the highest NIR fields by an angular distribution, which is peaked perpendicularly to both the XUV and NIR polarization directions. Experimental results are reproduced by a theoretical model based on the strong field approximation.

Design and test of a broadband split-and-delay unit for attosecond XUV-XUV pump-probe experiments

We present the design of a split-and-delay unit for the production of two delayed replicas of an incident extreme ultraviolet (XUV) pulse. The device features a single grazing incidence reflection in combination with attenuation of remaining infrared light co-propagating with the XUV beam, offering a high throughput without the need of introducing additional optics that would further decrease the XUV flux. To achieve the required spatial and temporal stabilities, the device is controlled by two PID-controllers monitoring the delay and the beam pointing using an optical reference laser beam, making collimation of the beam by additional optics unnecessary. Finally, we demonstrate the stability of the split-and-delay unit by performing all-reflective autocorrelation measurements on broadband few-cycle laser pulses.

Micro-Focusing of Broadband High-Order Harmonic Radiation by a Double Toroidal Mirror

We present an optical system based on two toroidal mirrors in a Wolter configuration to focus broadband XUV radiation. Optimization of the focusing optics alignment is carried out with the aid of an XUV wavefront sensor. Back-propagation of the optimized wavefront to the focus yields a focal spot of 3.6

A Versatile Velocity Map Ion-Electron Covariance Imaging Spectrometer for High-Intensity XUV Experiments

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Macroscopic Optimization of High Harmonic Generation for High Power Laser Pulses

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