Extreme Ultraviolet Laser Research Articles

Demonstration of a kHz-repetition-rate extreme ultraviolet laser at 41.8 nm.

We demonstrate the operation of a plasma-based extreme ultraviolet (XUV) laser at a 1 kHz repetition rate driven by infrared pump pulses of less than 20 mJ. The 41.8 nm laser pulses were generated in a Xe plasma created by optical-field ionization by the L1 Allegra laser at ELI Beamlines. The output power of the XUV laser lies in the few microwatt range, and the energy efficiency of this pumping scheme opens the way for further scaling in repetition rate and average power.

Exploring photoionization of gas-phase free radicals with a widely tunable VUV laser at moderate spectral resolution

The VUv Laser for Considering Astrophysical and Isolated Molecules (VULCAIMs) setup [Harper et al., Phys. Chem. Chem. Phys. 24, 2777 (2022)] integrates a narrow-bandwidth tunable vacuum ultraviolet (VUV) and extreme ultraviolet (XUV) nanosecond-pulsed laser system (6–16 eV) and a photoelectron spectrometer, designed for recording high-spectral-resolution (rotationally resolved) photoelectron spectra of gas-phase free radicals. This approach usually needs beforehand medium-resolution synchrotron data to guide the selection of specific spectral regions to be investigated at higher resolution with the VULCAIM setup. We present an upgraded version of the VUV laser system integrating an optical parametric oscillator for continuously scanned medium-resolution measurements (<3 cm−1) across the whole VUV and XUV spectral ranges. This innovation enables broader coverage without the need to access synchrotron facilities. Furthermore, rapid mode switching allows for maintaining optimized radical production conditions from mid-resolution to high-resolution operation mode, enhancing spectroscopy capabilities significantly. The new capabilities of the VULCAIM setup are illustrated on two showcases of photoionization studies: the nitric oxide (NO) stable molecular species and the benzyl (C6H5CH2) free radical produced by pyrolysis.

Extreme ultraviolet laser ablation and time-of-flight mass spectrometry of gold, aluminum, and copper targets

Extreme ultraviolet laser ablation and time-of-flight mass spectrometry of gold, aluminum, and copper targets

Double diffraction imaging of x-ray induced structural dynamics in single free nanoparticles

Because of their high photon flux, x-ray free-electron lasers (FEL) allow to resolve the structure of individual nanoparticles via coherent diffractive imaging (CDI) within a single x-ray pulse. Since the inevitable rapid destruction of the sample limits the achievable resolution, a thorough understanding of the spatiotemporal evolution of matter on the nanoscale following the irradiation is crucial. We present a technique to track x-ray induced structural changes in time and space by recording two consecutive diffraction patterns of the same single, free-flying nanoparticle, acquired separately on two large-area detectors opposite to each other, thus examining both the initial and evolved particle structure. We demonstrate the method at the extreme ultraviolet (XUV) and soft x-ray Free-electron LASer in Hamburg (FLASH), investigating xenon clusters as model systems. By splitting a single XUV pulse, two diffraction patterns from the same particle can be obtained. For focus intensities of about 2×1012 W cm−2 we observe still largely intact clusters even at the longest delays of up to 650 picoseconds of the second pulse, indicating that in the highly absorbing systems the damage remains confined to one side of the cluster. Instead, in case of five times higher flux, the diffraction patterns show clear signatures of disintegration, namely increased diameters and density fluctuations in the fragmenting clusters. Future improvements to the accessible range of dynamics and time resolution of the approach are discussed.

The Role of Momentum Partitioning in Covariance Ion Imaging Analysis.

We present results from a covariance ion imaging study, which employs extensive filtering, on the relationship between fragment momenta to gain deeper insight into photofragmentation dynamics. A new data analysis approach is introduced that considers the momentum partitioning between the fragments of the breakup of a molecular polycation to disentangle concurrent fragmentation channels, which yield the same ion species. We exploit this approach to examine the momentum exchange relationship between the products, which provides direct insight into the dynamics of molecular fragmentation. We apply these techniques to extensively characterize the dissociation of 1-iodopropane and 2-iodopropane dications prepared by site-selective ionization of the iodine atom using extreme ultraviolet intense femtosecond laser pulses with a photon energy of 95 eV. Our assignments are supported by classical simulations, using parameters largely obtained directly from the experimental data.

Azimuthally extreme-ultraviolet focal splitter by modified spiral photon sieves

Extreme Ultraviolet (EUV) radiation is a short-wavelength light source that has important applications in many fields, such as optical communication, particle manipulation, and ultrahigh resolution imaging. However, the highly absorptive nature of EUV light makes it challenging to design suitable focusing optics, such as focal splitters, to properly manipulate the energetic light. Here, we propose modified spiral photon sieves to transform EUV laser light into azimuthally splitting focusing. A genetic algorithm was used to design and optimize the azimuthally focal splitters. A capillary discharge EUV laser at 46.9 nm was used to verify the effectiveness of our proposed method, and PMMA targets were used to record the focused laser spot. The profile of the recorded patterns measured by atomic force microscopy shows that the focal spots in the experiment are diffraction-limited and agreed with the theoretical analysis. The proposed technique provides a new way for manipulating EUV light and further extends the applications ranging from EUV to soft x rays.

A high-efficiency programmable modulator for extreme ultraviolet light with nanometre feature size based on an electronic phase transition

AbstractThe absence of efficient light modulators for extreme ultraviolet (EUV) and X-ray photons considerably limits their real-life application, particularly when even slight complexity of the beam patterns is required. Here we report on a novel approach to reversible imprinting of a holographic mask in an electronic Wigner crystal material with a sub-90-nm feature size. The structure is imprinted on a sub-picosecond timescale using EUV laser pulses, and acts as a high-efficiency diffraction grating that deflects EUV or soft X-ray light. The imprinted nanostructure is stable after the removal of the exciting beams at low temperatures, but can be easily erased by a single heating beam. Modelling shows that the efficiency of the device can exceed 1%, approaching state-of-the-art etched gratings, but with the benefit of being programmable and tunable over a large range of wavelengths. The observed effect is based on the rapid change of lattice constant upon transition between metastable electronically ordered phases in a layered transition metal dichalcogenide. The proposed approach is potentially useful for creating tunable light modulators in the EUV and soft X-ray spectral ranges.

Free light-shape focusing in extreme-ultraviolet radiation with self-evolutionary photon sieves

Extreme-ultraviolet (EUV) radiation is a promising tool, not only for probing microscopic activities but also for processing nanoscale structures and performing high-resolution imaging. In this study, we demonstrate an innovative method to generate free light-shape focusing with self-evolutionary photon sieves under a single-shot coherent EUV laser; this includes vortex focus shaping, array focusing, and structured-light shaping. The results demonstrate that self-evolutionary photon sieves, consisting of a large number of specific pinholes fabricated on a piece of Si3N4 membrane, are capable of freely regulating an EUV light field, for which high-performance focusing elements are extremely lacking, let alone free light-shape focusing. Our proposed versatile photon sieves are a key breakthrough in focusing technology in the EUV region and pave the way for high-resolution soft X-ray microscopy, spectroscopy in materials science, shorter lithography, and attosecond metrology in next-generation synchrotron radiation and free-electron lasers.

Bond dissociation energy of N2 measured by state-to-state resolved threshold fragment yield spectra.

The precise determination of the bond dissociation energy of N2 is crucial for thermochemistry database and theoretical calculations. However, there has been ongoing debate regarding its exact value. In this study, we used the velocity map imaging method combined with an extreme ultraviolet laser to measure the threshold fragment yield (TFY) spectra of N2 in the N(2D) + N(2D) photodissociation channels. By integrating the signals within a small circular area on the fragment velocity map images, we were able to obtain TFY spectra at nine different dissociation thresholds. These spectra are rotational state-resolved for the N2(J″) molecules and spin-orbit state-resolved for the dissociation channels involving N(2D) fragments. By employing the Wigner threshold law to simulate the TFY spectra and conducting statistical analysis on the comprehensive dataset, we determined the N2 bond dissociation energy to be 78 691.09 ± 0.15cm-1. This work now places N2 among the few diatomic molecules with bond dissociation energies measured at sub-wavenumber precision.

Time‐Resolved Photoemission Electron Microscopy on a ZnO Surface Using an Extreme Ultraviolet Attosecond Pulse Pair

AbstractElectrons photoemitted by extreme ultraviolet attosecond pulses derive spatially from the first few atomic surface layers and energetically from the valence band and highest atomic orbitals. As a result, it is possible to probe the emission dynamics from a narrow 2D region in the presence of optical fields, as well as obtain elemental specific information. However, combining this with spatially‐resolved imaging is a long‐standing challenge because of the large inherent spectral width of attosecond pulses, as well as the difficulty of making them at high repetition rates. Here, this work demonstrates an attosecond interferometry experiment on a zinc oxide (ZnO) surface using spatially and energetically resolved photoelectrons. Photoemission electron microscopy is combined with near‐infrared pump ‐ extreme ultraviolet probe laser spectroscopy and the instantaneous phase of an infrared field is resolved with high spatial resolution. Results show how the core level states with low binding energy of ZnO are well suited to perform spatially resolved attosecond interferometry experiments. A distinct phase shift of the attosecond beat signal is observed across the laser focus which is attributed to wavefront differences between the pump and the probe fields at the surface. This work demonstrates a clear pathway for attosecond interferometry with high spatial resolution at atomic scale surface regions opening up for a detailed understanding of nanometric light‐matter interaction.

Study on electron response to near-infrared, ultraviolet and extreme ultraviolet femtosecond laser by first-principle

The phenomenon of laser-induced electronic evolution in semiconductors is an essential issue in laser fabrication, which has been extensively investigated within the near-infrared and visible spectral ranges. However, electronic evolution at short wavelength laser has neither been systematically investigated. In this paper, time-dependent density functional theory is employed to investigate the response in silicon under laser irradiation of different wavelengths. The result shows that shorter wavelength induces the excitation of electrons to higher energy levels, consequently leading to increased impact ionization rates. Such a moderate excitation of energetic electrons even at low-medium intensity is considered as a distinctive feature of extreme ultraviolet light laser, which is expected to further enhance the quality of laser processing.

Electron vortices generation of photoelectron of H2+ by counter-rotating circularly polarized attosecond pulses

Molecular-frame photoelectron momentum distributions (MF-PMDs) of an H2+ molecule ion in the presence of a pair of counter-rotating circularly polarized attosecond extreme ultraviolet laser pulses is studied by numerically solving the two-dimensional time-dependent Schrödinger equation within the frozen-nuclei approximation. At small time delay, our simulations show that the electron vortex structure is sensitive to the time delay and relative phase between the counter-rotating pulses when they are partially overlapped. By adjusting time delay and relative phase, we have the ability to manipulate the MF-PMDs and the appearance of spiral arms. We further show that the internuclear distance can affect the spiral vortices due to its different transition cross sections in the parallel and perpendicular geometries. The lowest-order perturbation theory is employed to interpret these phenomena qualitatively. It is concluded that the internuclear distance-dependent transition cross sections and the confinement effect in diatomic molecules are responsible for the variation of vortex structures in the MF-PMDs.

Imaging and Controlling Ultrafast Electron Pulses Emitted from Plasmonic Nanostructures.

We experimentally study photoemission from gold nanodisk arrays using space-, time-, and energy-resolved photoemission electron microscopy. When excited by a plasmonic resonant infrared (IR) laser pulse, plasmonic hotspots are generated owing to local surface plasmon resonance. Photoelectrons emitted from each plasmonic hotspot form a nanoscale and ultrashort electron pulse. When the system is excited by an extreme ultraviolet (EUV) laser pulse, a uniformly distributed photoelectron cloud is formed across the sample surface. When excited by the IR and EUV laser pulses together, both the photoemission image and kinetic energy vary significantly for the IR laser-generated electrons depending on the time delay between the two laser pulses. These observations are well explained by the Coulomb interaction with the EUV laser-generated electron cloud. Our study offers a feasible approach to manipulate the energy of electron pulse emitted from a plasmonic nanostructure on an ultrafast time scale.

Generation of collimated extreme ultraviolet radiation by single-photon process

Generating laser with short wavelength is a bottleneck problem in laser technology. The current applicable table-top extreme ultraviolet (EUV) lasers are all generated by multi-photon process with low efficiency. By utilizing metastable helium atoms excited by microwave and irradiated by a resonant laser, here we report the development of 58.4 nm collimated radiation by single-photon-excitation related anti-Stokes Raman scattering (ASRS). The conversion efficiency is much higher than that of high harmonic generation (HHG). The same divergence of 1.4 mrad as that of excitation laser indicates its stimulating character. Our results show an applicable path towards up-conversion by single-photon process to generate table-top EUV lasers.

Focusing and Wavefront Splitting of an Extreme Ultraviolet Laser with a Tubular Optical Element

A capillary discharge extreme ultraviolet laser is focused and wavefront split at 46.9 nm by a tubular optical element. The reflectivity at 46.9 nm is both simulated and measured to be higher than 90% with a slight optical aberration. The operating principle of the tubular element for focusing and wavefront splitting is discussed. Dense and intense grating-like fringes with a period of ~150 nm are achieved. The method used in this work allows nano-scale processing with extreme ultraviolet laser at single-shot exposure mode.

Ultrafast Roaming Mechanisms in Ethanol Probed by Intense Extreme Ultraviolet Free-Electron Laser Radiation: Electron Transfer versus Proton Transfer

Ultrafast H2+ and H3+ formation from ethanol is studied using pump-probe spectroscopy with an extreme ultraviolet (XUV) free-electron laser. The first pulse creates a dication, triggering H2 roaming that leads to H2+ and H3+ formation, which is disruptively probed by a second pulse. At photon energies of 28 and 32 eV, the ratio of H2+ to H3+ increases with time delay, while it is flat at a photon energy of 70 eV. The delay-dependent effect is ascribed to a competition between electron and proton transfer. High-level quantum chemistry calculations show a flat potential energy surface for H2 formation, indicating that the intermediate state may have a long lifetime. The ab initio molecular dynamics simulation confirms that, in addition to the direct emission, a small portion of H2 undergoes a roaming mechanism that leads to two competing pathways: electron transfer from H2 to C2H4O2+ and proton transfer from C2H4O2+ to H2.

FLASH and the FLASH2020+ project—current status and upgrades for the free-electron laser in Hamburg at DESY

The free-electron laser in Hamburg, FLASH, is the first extreme ultra-violet and soft X-ray free-electron laser (FEL) user facility and has been continuously upgraded since its start in 2005. Further major works are currently underway within the FLASH2020+ project that pioneeringly implements full repetition rate external seeding at a superconducting accelerator facility. With fully tunable undulators providing variable polarization FEL pulses, we expect FLASH to turn into the ideal spectroscopy machine for ultrafast processes within the coming years.

Photon Acceleration from Optical to XUV.

The propagating density gradients of a plasma wakefield may frequency upshift a trailing witness laser pulse, a process known as "photon acceleration." In uniform plasma, the witness laser will eventually dephase because of group delay. We find phase-matching conditions for the pulse using a tailored density profile. An analytic solution for a 1D nonlinear plasma wake with an electron beam driver indicates that, even though the plasma density decreases, the frequency shift reaches no asymptotic limit, i.e., is unlimited provided the wake can be sustained. In fully self-consistent 1D particle-in-cell (PIC) simulations, more than 40 times frequency shifts were demonstrated. In quasi-3D PIC simulations, frequency shifts up to 10 times were observed, limited only by simulation resolution and nonoptimized driver evolution. The pulse energy increases in this process, by a factor of 5, and the pulse is guided and temporally compressed by group velocity dispersion, resulting in the resulting extreme ultraviolet laser pulse having near-relativistic (a_{0}∼0.4) intensity.

Capturing transient core-to-core resonances in Kr in intense extreme-ultraviolet laser fields by electron-ion coincidence spectroscopy

Resonances between core-hole states have been long hypothesized to understand dynamics of atoms and molecules exposed to intense XFEL pulses, but evaded clear identification due to their transient nature. The authors report clear evidence of core-to-core resonances by electron-ion coincidence spectroscopy on Kr atoms and elucidate the importance in nonlinear electronic responses of matter to high-frequency laser fields.

FLASH free electron laser pump-probe laser concept based on spectral broadening of high-power ytterbium picosecond systems in multi-pass cells.

Within the FLASH2020+ upgrade, the pump-probe laser capabilities of the extreme ultraviolet and soft x-ray free-electron laser (XFEL) FLASH in Hamburg will be extended. In particular, providing wavelength tunability, shorter pulse durations, and reduced arrival time jitter will increase the scientific opportunities and the time resolution for the XFEL-optical laser pump-probe experiments. We present here a novel concept for the pump-probe laser at FLASH that is based on the post-compression of picosecond pulses emitted from high-power Ytterbium:YAG slab amplifiers. Flexible reduction of the pulse duration is facilitated by spectral broadening in pressure-tunable multi-pass cells. As an application, we show the pumping of a commercial optical parametric amplifier with 150fs post-compressed pulses. By means of an additional difference frequency generation stage, tunable spectral coverage from 1.3 to 16μm is reached with multi-μJ, sub-150fs pulses. Finally, a modular reconfiguration approach to the optical setups close to the free-electron laser instruments is implemented. This enables fast installation of the nonlinear frequency converters at the end stations for user operation and flexibility between different instruments in the two experimental halls.