High-order Harmonic Generation Source Research Articles

High-flux wavelength tunable XUV source in the 12-40.8 eV photon energy range with adjustable energy and time resolution for Tr-ARPES applications.

High-order harmonic generation (HHG) has a broad spectrum covering vacuum ultraviolet to extreme ultraviolet (XUV) bands, which is useful for applications involving material analyses at different information depths. Such an HHG light source is perfect for time- and angle-resolved photoemission spectroscopy. Here, we demonstrate a high-photon flux HHG source driven by a two-color field. Applying a fused silica compression stage to reduce the driving pulse width, we obtained a high XUV photon flux of 2 × 1012 phs/s @21.6 eV on target. We designed a classical diffraction mounted (CDM) grating monochromator that can achieve a wide range of photon energy from 12 to 40.8 eV, while the time resolution is improved by reducing the pulse front tilt after the harmonic selection. We designed a spatial filtering method to adjust the time resolution using the CDM monochromator and significantly reduced the pulse front tilt of the XUV pulses. We also demonstrate a detailed prediction of the energy resolution broadening which is caused by the space charge effect.

High-harmonic generation from artificially stacked 2D crystals

Abstract We report a coherent layer-by-layer build-up of high-order harmonic generation (HHG) in artificially stacked transition metal dichalcogenides (TMDC) crystals in their various stacking configurations. In the experiments, millimeter-sized single crystalline monolayers are synthesized using the gold foil-exfoliation method, followed by artificially stacking on a transparent substrate. High-order harmonics up to the 19th order are generated by the interaction with a mid-infrared (MIR) driving laser. We find that the generation is sensitive to both the number of layers and their relative orientation. For AAAA stacking configuration, both odd- and even-orders exhibit a quadratic increase in intensity as a function of the number of layers, which is a signature of constructive interference of high-harmonic emission from successive layers. Particularly, we observe some deviations from this scaling at photon energies above the bandgap, which is explained by self-absorption effects. For AB and ABAB stacking, even-order harmonics remain below the detection level, consistent with the presence of inversion symmetry. Our study confirms our capability of producing nonperturbative high-order harmonics from stacked layered materials subjected to intense MIR fields without damaging samples. Our results have implications for optimizing solid-state HHG sources at the nanoscale and developing high-harmonics as an ultrafast probe of artificially stacked layered materials. Because the HHG process is a strong-field driven process, it has the potential to probe high-momentum and energy states in the bandstructure combined with atomic-scale sensitivity in real space, making it an attractive probe of novel material structures such as the Moiré pattern.

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 40eV 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.

Extreme-ultraviolet frequency combs for precision metrology and attosecond science

Femtosecond mode-locked lasers producing visible/infrared frequency combs have steadily advanced our understanding of fundamental processes in nature. For example, optical clocks employ frequency-comb techniques for the most precise measurements of time, permitting the search for minuscule drifts of natural constants. Furthermore, the generation of extreme-ultraviolet attosecond bursts synchronized to the electric field of visible/infrared femtosecond pulses affords real-time measurements of electron dynamics in matter. Cavity-enhanced high-order harmonic generation sources uniquely combine broadband vacuum- and extreme-ultraviolet spectral coverage with multimegahertz pulse repetition rates and coherence properties akin to those of frequency combs. Here we review the coming of age of this technology and its recent applications and prospects, including precision frequency-comb spectroscopy of electronic and potentially nuclear transitions, and low-space-charge attosecond-temporal-resolution photoelectron spectroscopy with nearly 100% temporal detection duty cycle. This Review covers the milestones for extreme-ultraviolet frequency combs and their applications. A future impact on the construction of nuclear-based optical clocks and multidimensional attosecond photoelectron spectroscopy of solids is remarked.

Off-resonance-enhanced polarization control in two-color atomic ionization

We investigate a polarization control scheme in two-color two-photon atomic ionization. Experiments employing free-electron laser or high-order harmonic generation sources have shown light polarization dependencies in above threshold ionization of atoms assisted with an IR field. These were mostly performed at relatively high photoelectron energies where the soft-photon approximation remains valid. We use here a perturbation theory approach to show the larger degree of control that can be attained when the short wavelength photon energy is below the ionization threshold. This largely unexplored energy region offers unique possibilities to achieve polarization control of the reaction.

Singleshot polychromatic coherent diffractive imaging with a high-order harmonic source.

Singleshot polychromatic coherent diffractive imaging is performed with a high-intensity high-order harmonic generation source. The coherence properties are analyzed and several reconstructions show the shot-to-shot fluctuations of the incident beam wavefront. The method is based on a multi-step approach. First, the spectrum is extracted from double-slit diffraction data. The spectrum is used as input to extract the monochromatic sample diffraction pattern, then phase retrieval is performed on the quasi-monochromatic data to obtain the sample's exit surface wave. Reconstructions based on guided error reduction (ER) and alternating direction method of multipliers (ADMM) are compared. ADMM allows additional penalty terms to be included in the cost functional to promote sparsity within the reconstruction.

Extreme ultraviolet time- and angle-resolved photoemission setup with 21.5 meV resolution using high-order harmonic generation from a turn-key Yb:KGW amplifier.

Characterizing and controlling electronic properties of quantum materials require direct measurements of nonequilibrium electronic band structures over large regions of momentum space. Here, we demonstrate an experimental apparatus for time- and angle-resolved photoemission spectroscopy using high-order harmonic probe pulses generated by a robust, moderately high power (20 W) Yb:KGW amplifier with a tunable repetition rate between 50 and 150 kHz. By driving high-order harmonic generation (HHG) with the second harmonic of the fundamental 1025 nm laser pulses, we show that single-harmonic probe pulses at 21.8 eV photon energy can be effectively isolated without the use of a monochromator. The on-target photon flux can reach 5 × 1010 photons/s at 50 kHz, and the time resolution is measured to be 320 fs. The relatively long pulse duration of the Yb-driven HHG source allows us to reach an excellent energy resolution of 21.5 meV, which is achieved by suppressing the space-charge broadening using a low photon flux of 1.5 × 108 photons/s at a higher repetition rate of 150 kHz. The capabilities of the setup are demonstrated through measurements in the topological semimetal ZrSiS and the topological insulator Sb2-xGdxTe3.

Resonant Faraday effect using high-order harmonics for the investigation of ultrafast demagnetization

During the past few years high-order harmonic generation (HHG) has opened up the field of ultrafast spectroscopy to an ever larger community by providing a table-top and affordable femtosecond extreme ultraviolet (EUV) and soft-x-ray source. In particular, the field of femtomagnetism has largely benefited from the development of these sources. However, the use of x-ray magnetic circular dichroism (XMCD) as a probe of magnetization, the most versatile and reliable one, has been constrained by the lack of polarization control at HHG sources, so studies have relied on more specific magneto-optical effects. Even the recent developments on the generation of elliptically polarized harmonics have only resulted in a few time-resolved experiments relying on this powerful technique since they add complexity to already-difficult measurements. In this article we show how to easily probe magnetization dynamics with linearly polarized EUV or soft-x-ray light with a versatility similar to XMCD by exploiting the Faraday effect. Static and time-resolved measurements of the Faraday effect are presented around the Co $M$ edges. Using simple theoretical considerations, we show how to retrieve the samples magnetization dynamics from the Faraday rotation and ellipticity transients. Ultrafast demagnetization dynamics of a few nanometers in Co-based samples are measured with this method in out-of-plane as well as in-plane magnetization configurations, showing its great potential for the study of femtomagnetism.

Quasi-phase-matched high-harmonic generation in gas-filled hollow-core photonic crystal fiber

High-order harmonic generation (HHG) provides a promising tabletop source of coherent short wavelength radiation. However, the low generation efficiency limits the mean photon flux of HHG sources when driven with low average power, kHz repetition rate lasers. The HHG flux could be increased by employing MHz repetition rate driving lasers. However, the low pulse energy necessitates tight focusing, which limits the effective interaction volume. Generating harmonics in a gas-filled photonic crystal fiber (PCF) mitigates this problem, but for both free focus and PCF targets, the HHG conversion efficiency is optimized at technologically challenging multibar gas pressures. Here, we perform HHG with μJ-level driving pulses in a hollow-core PCF. We observe dramatic 60-fold enhancement of the HHG flux through a time-multiplexed multimodal quasi-phase-matching technique at low gas pressures. We also observe high harmonic photon energies up to 61.6 eV with continuous spectral tunability made possible by controlled ionization-induced blue shifting of the driving laser.

Multiple ionization of argon via multi-XUV-photon absorption induced by 20-GW high-order harmonic laser pulses

We report the observation of multiple ionization of argon through multi-XUV-photon absorption induced by an unprecedentedly powerful laser driven high-order harmonic generation source. Comparing the measured intensity dependence of the yield of the different argon charge states with numerical calculations we can infer the different channels---direct and sequential---underlying the interaction. While such studies were feasible so far only with free electron laser (FEL) sources, this paper connects highly nonlinear XUV processes with the ultrashort time scales inherent to the harmonic pulses and highlights the advanced perspectives of emerging large scale laser research infrastructures.

Compact 200 kHz HHG source driven by a few-cycle OPCPA

We present efficient high-order harmonic generation (HHG) based on a high-repetition rate, few-cycle, near infrared (NIR), carrier-envelope phase stable, optical parametric chirped pulse amplifier (OPCPA), emitting 6 fs pulses with 9 μJ pulse energy. In krypton, we reach conversion efficiencies from the NIR to the extreme ultraviolet (XUV) radiation pulse energy on the order of ∼10−6 with less than 3 μJ driving pulse energy. This is achieved by optimizing the OPCPA for a spatially and temporally clean pulse and by a specially designed high-pressure gas target. In the future, the high efficiency of the HHG source will be beneficial for high-repetition rate two-colour (NIR-XUV) pump-probe experiments, where the available pulse energy from the laser has to be distributed economically between pump and probe pulses.

Performance of a ruthenium beam separator used to separate soft x rays from light generated by a high-order harmonic light source.

We describe the design and fabrication of a ruthenium beam separator used to simultaneously attenuate infrared light and reflect soft x rays. Measurements in the infrared and soft x-ray regions showed the beam separator to have a reflectivity of 50%-85% in the wavelength region from 6 to 10 nm at a grazing incidence angle of 7.5 deg and 4.3% at 800 nm and the same angle of grazing incidence, indicating that the amount of attenuation is 0.05-0.09. These results show that this beam separator could provide an effective means for separating IR light from soft x rays in light generated by high-order harmonic generation sources.

Advances in high-order harmonic generation sources for time-resolved investigations

We review the main research directions ongoing in the development of extreme ultraviolet sources based on high-harmonic generation for the synthesization and application of trains and isolated attosecond pulses to time-resolved spectroscopy. A few experimental and theoretical works will be discussed in connection to well-established attosecond techniques. In this context, we present the unique possibilities offered for time-resolved investigations on the attosecond timescale by the new Extreme Light Infrastructure Attosecond Light Pulse Source, which is currently under construction.

Real-time fragmentation dynamics of clusters ionized by intense extreme-ultraviolet pulses

We investigate the fragmentation dynamics of atomic clusters ionized by intense extreme-ultraviolet pulses from a high-order harmonic generation source. It is demonstrated that the transient modification of the trimer fragment yield induced by a weak near-infrared (NIR) probe pulse provides valuable information on the cluster disintegration process. For medium-sized Ar clusters and delays of around 5 ps, we observe a transition from a collective response, where efficient absorption of the NIR laser energy takes place, to a state where the interaction of the probe laser pulse with individual fragments dominates. The cluster disintegration is faster for smaller clusters, in agreement with a simple physical picture taking into account the measured expansion speeds of excited and ionic fragments. For Xe clusters, we find a significantly increased fragmentation time of about 40 ps, attributed to the larger atomic mass and to more efficient electron–ion recombination processes.

Coherent diffractive imaging microscope with a high-order harmonic source.

We report the generation of highly coherent extreme ultraviolet sources with wavelengths around 30 and 10 nm by phase-matched high-order harmonic generation (HHG) in a gas cell filled with argon and helium, respectively. We then perform coherent diffractive imaging (CDI) by using a focused narrow-bandwidth HHG source with wavelength around 30 nm as an illumination beam for two kinds of samples. The first is a transmission sample and the second is a absorption sample. In addition, we report the successful reconstruction of a complex absorption sample using a tabletop high-harmonic source. This will open the path to the realization of a compact soft x-ray microscope to investigate biological samples such as membrane proteins.

Femtosecond-laser–induced modifications in Co/Pt multilayers studied with tabletop resonant magnetic scattering

We characterize the magnetic domain structure of Co/Pt multilayer films on length scales below one hundred nanometers using resonant magnetic scattering and magnetic force microscopy. The extreme ultraviolet light for the scattering experiment is created by a laser-based high-order harmonic generation source. After illumination with intense ultrashort infrared laser pulses, we observe pronounced changes in the magnetic structure and morphology. This study points out the importance of a detailed analysis of the different laser-induced modifications of a magnetic thin film that influence the scattering patterns.

High-harmonic phase spectroscopy using a binary diffractive optical element

We report on high-order harmonic generation (HHG) using a Ti:sapphire laser beam phase shaped with a binary diffractive optical element (DOE) to create two spatially separated synchronized HHG sources at the focus of a lens. Using full three-dimensional computations, we show numerically that the harmonic dipole phase is imprinted in the resulting far-field fringe pattern. Using the corresponding experimental arrangement, we measure HHG phase in aligned carbon dioxide. This arrangement is robust, extremely stable, simple to use, and gives highly resolved fringes. It thus opens new perspectives for combined and refined HHG phase measurements in excited samples.

Development of Coherent Extreme-Ultraviolet Scatterometry Microscope with High-Order Harmonic Generation Source for Extreme-Ultraviolet Mask Inspection and Metrology

In extreme-ultraviolet (EUV) lithography, defect-free mask production is one of the critical issues for the high-volume manufacturing of semiconductor devices. We developed a coherent EUV scatterometry microscope (CSM), which is a simple lensless system. The CSM records diffraction from mask patterns with a charge-coupled-device (CCD) camera directly, which is illuminated with a coherent EUV light. Since a practical standalone system is required by the industry, we developed a standalone CSM system employing a high-order harmonic generation (HHG) EUV source. The 59th high-order harmonic generation of 13.5 nm wavelength is pumped by a tabletop, 6 mJ, 32 fs, Ti:sapphire laser system. The EUV output energy of 1 µW is successfully achieved. We performed the observation of an EUV mask using the HHG-CSM system. The detection limit of the line defect size is improved to 2 nm for the high output power of the HHG EUV source.

Development of Coherent Extreme-Ultraviolet Scatterometry Microscope with High-Order Harmonic Generation Source for Extreme-Ultraviolet Mask Inspection and Metrology

In extreme-ultraviolet (EUV) lithography, defect-free mask production is one of the critical issues for the high-volume manufacturing of semiconductor devices. We developed a coherent EUV scatterometry microscope (CSM), which is a simple lensless system. The CSM records diffraction from mask patterns with a charge-coupled-device (CCD) camera directly, which is illuminated with a coherent EUV light. Since a practical standalone system is required by the industry, we developed a standalone CSM system employing a high-order harmonic generation (HHG) EUV source. The 59th high-order harmonic generation of 13.5 nm wavelength is pumped by a tabletop, 6 mJ, 32 fs, Ti:sapphire laser system. The EUV output energy of 1 µW is successfully achieved. We performed the observation of an EUV mask using the HHG-CSM system. The detection limit of the line defect size is improved to 2 nm for the high output power of the HHG EUV source.

Femtosecond time-resolved photoelectron spectroscopy with a vacuum-ultraviolet photon source based on laser high-order harmonic generation

A laser-based tabletop approach to femtosecond time-resolved photoelectron spectroscopy with photons in the vacuum-ultraviolet (VUV) energy range is described. The femtosecond VUV pulses are produced by high-order harmonic generation (HHG) of an amplified femtosecond Ti:sapphire laser system. Two generations of the same setup and results from photoelectron spectroscopy in the gas phase are discussed. In both generations, a toroidal grating monochromator was used to select one harmonic in the photon energy range of 20-30 eV. The first generation of the setup was used to perform photoelectron spectroscopy in the gas phase to determine the bandwidth of the source. We find that our HHG source has a bandwidth of 140 ± 40 meV. The second and current generation is optimized for femtosecond pump-probe photoelectron spectroscopy with high flux and a small spot size at the sample of the femtosecond probe pulses. The VUV radiation is focused into the interaction region with a toroidal mirror to a spot smaller than 100 × 100 μm(2) and the flux amounts to 10(10) photons/s at the sample at a repetition rate of 1 kHz. The duration of the monochromatized VUV pulses is determined to be 120 fs resulting in an overall pump-probe time resolution of 135 ± 5 fs. We show how this setup can be used to map the transient valence electronic structure in molecular dissociation.