Christoph Heyl

High-order harmonic generation with mu J laser pulses at high repetition rates

We investigate the generation of high-order harmonics using laser pulse energies in the few-μJ range at high repetition rates. We analyse how the conversion efficiency is influenced by the tight focusing geometry required for the generation of high-order harmonics under these conditions. A generalized phase-matching model allows us to discuss macroscopic phase effects independent of focal length. We present experimental results using the example of a 100 kHz laser system to generate harmonics up to the 27th order in Ar with a photon flux up to 3 × 109 photons s−1 into one harmonic order. High-repetition-rate femtosecond or even attosecond light sources open new possibilities for a broad range of applications such as time-resolved photoelectron spectroscopy and microscopy in the extreme ultraviolet regime.

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.

Scale-invariant nonlinear optics in gases

Nonlinear optical methods have become ubiquitous in many scientific areas, from fundamental studies of time-resolved electron dynamics to microscopy and spectroscopy applications. They are, however, often limited to a certain range of parameters such as pulse energy and average power. Restrictions arise from, for example, the required field intensity as well as from parasitic nonlinear effects and saturation mechanisms. Here, we identify a fundamental principle of nonlinear light–matter interaction in gases and show that paraxial nonlinear wave equations are scale-invariant if spatial dimensions, gas density, and laser pulse energy are scaled appropriately. As an example, we apply this principle to high-order harmonic generation and provide a general method for increasing peak and average power of attosecond sources. In addition, we experimentally demonstrate the implications for the compression of short laser pulses. Our scaling principle extends well beyond those examples and includes many nonlinear processes with applications in different areas of science.

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.

Noncollinear optical gating

We present a novel scheme for high-order harmonic generation, enabling the production of spatially separated isolated attosecond pulses. This can be achieved by driving the generation process with two identical, but temporally delayed laser pulses, which are noncollinearly overlapping in the generation medium. Our approach provides intense attosecond pulses directly separated from the fundamental field, which is left undistorted. The method is therefore ideally suited for pump-probe studies in the extreme ultraviolet regime and promises new advances for intra-cavity attosecond pulse generation. We present a theoretical description of noncollinear optical gating, with an analytical derivation and simulations using the strong field approximation.

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.

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.

Introduction to macroscopic power scaling principles for high-order harmonic generation

This tutorial presents an introduction to power scaling concepts for high-order harmonic generation (HHG) and attosecond pulse production. We present an overview of state-of-the-art HHG-based extreme ultraviolet (XUV) sources, followed by a brief introduction to basic principles underlying HHG and a detailed discussion of macroscopic effects and scaling principles. Particular emphasis is put on a general scaling model that allows the invariant scaling of the HHG process both, to μJ-level driving laser pulses and thus to multi-MHz repetition rates as well as to 100 mJ-or even Joule-level laser pulses, allowing new intensity regimes with attosecond XUV pulses.

Roadmap on ultrafast optics

The year 2015 marked the 25th anniversary of modern ultrafast optics, since the demonstration of the first Kerr lens modelocked Ti:sapphire laser in 1990 (Spence et al 1990 Conf. on Lasers and Electro-Optics, CLEO, pp 619–20) heralded an explosion of scientific and engineering innovation. The impact of this disruptive technology extended well beyond the previous discipline boundaries of lasers, reaching into biology labs, manufacturing facilities, and even consumer healthcare and electronics. In recognition of such a milestone, this roadmap on Ultrafast Optics draws together articles from some of the key opinion leaders in the field to provide a freeze-frame of the state-of-the-art, while also attempting to forecast the technical and scientific paradigms which will define the field over the next 25 years. While no roadmap can be fully comprehensive, the thirteen articles here reflect the most exciting technical opportunities presented at the current time in Ultrafast Optics. Several articles examine the future landscape for ultrafast light sources, from practical solid-state/fiber lasers and Raman microresonators to exotic attosecond extreme ultraviolet and possibly even zeptosecond x-ray pulses. Others address the control and measurement challenges, requiring radical approaches to harness nonlinear effects such as filamentation and parametric generation, coupled with the question of how to most accurately characterise the field of ultrafast pulses simultaneously in space and time. Applications of ultrafast sources in materials processing, spectroscopy and time-resolved chemistry are also discussed, highlighting the improvements in performance possible by using lasers of higher peak power and repetition rate, or by exploiting the phase stability of emerging new frequency comb sources.