Extreme Ultraviolet Laser Research Articles

Enhanced Nonlinear Double Excitation of He in Intense Extreme Ultraviolet Laser Fields

Nonlinear, three-photon double excitation of He in intense extreme ultraviolet free-electron laser fields (∼24.1 eV, ∼5 TW/cm2) is presented. Resonances to the doubly excited states converging to the He+ N=3 level are revealed by the shot-by-shot photoelectron spectroscopy and identified by theoretical calculations based on the time-dependent Schrödinger equation for the two-electron atom under a laser field. It is shown that the three-photon double excitation is enhanced by intermediate Rydberg states below the first ionization threshold, giving a greater contribution to the photoionization yields than the two-photon process by more than 1 order of magnitude.

Coherent x-ray generation from below-threshold harmonics

The possibility of x-ray emission employing below-threshold-harmonic generation in the nontunneling regime is considered. The interaction of a tightly bound valence electron in a highly charged ion with intense extreme-ultraviolet laser radiation is investigated in the weakly relativistic regime by numerical solution of the two-dimensional relativistically corrected Schr\odinger equation. Nondipole effects and the relativistic mass correction are taken into account by expansion of the total Klein-Gordon Hamiltonian up to the second order in the ratio between the electron velocity and the speed of light. The harmonics below the ionization energy of the tightly bound system are found to be emitted with much higher probability than the standard plateau harmonics of loosely bound systems in the tunneling ionization regime for the same photon energy. This paves a path toward coherent hard x rays.

High-brightness optical-field-ionization collisional-excitation extreme-ultraviolet lasing pumped by a 100-TW laser system in an optically preformed plasma waveguide

Recent study on optical-field-ionization collisional-excitation extreme-ultraviolet lasing of Ni-like krypton at 32.8 nm pumped by a 100-TW laser system with an optically preformed plasma waveguide is reported. By using a 9-mm-long pure krypton plasma waveguide fabricated with the axicon-ignitor-heater scheme, the 32.8-nm extreme-ultraviolet laser provided an average output of 1012 photons/pulse at pump energy of 1 J, more than one order of magnitude enhancement relative to the previous results with the same scheme at pump energy of 235 mJ. It is also found the far-field pattern of laser beams varies from a single peak profile at low pump energy to an annular profile at high pump energy due to over-ionization of krypton ions at the center of the plasma channel.

Analysis of a scheme for de-magnified Talbot lithography

The authors describe a photolithographic scheme based on the replication of a periodic transparent mask in a photoresist utilizing the coherent self-imaging Talbot effect. A periodic two-dimensional diffractive structure (or Talbot mask) composed of unit tiles distributed in a square matrix was illuminated by a coherent extreme ultraviolet (EUV) beam from a table top EUV laser. The illumination beam was reflected in a spherical mirror and the Talbot mask was placed in the path of the convergent beam. At designed locations determined by the Talbot distance, reduced replicas of the mask were obtained and used to print the slightly de-magnified copies of the mask on the surface of a photoresist. Experimental results showing the de-magnification effect are in good agreement with the diffraction theory. The limits of the technique are discussed.

A flexible apparatus for attosecond photoelectron spectroscopy of solids and surfaces

We describe an apparatus for attosecond photoelectron spectroscopy of solids and surfaces, which combines the generation of isolated attosecond extreme-ultraviolet (XUV) laser pulses by high harmonic generation in gases with time-resolved photoelectron detection and surface science techniques in an ultrahigh vacuum environment. This versatile setup provides isolated attosecond pulses with photon energies of up to 140 eV and few-cycle near infrared pulses for studying ultrafast electron dynamics in a large variety of surfaces and interfaces. The samples can be prepared and characterized on an atomic scale in a dedicated flexible surface science end station. The extensive possibilities offered by this apparatus are demonstrated by applying attosecond XUV pulses with a central photon energy of ∼125 eV in an attosecond streaking experiment of a xenon multilayer grown on a Re(0001) substrate.

Evaluation of lab-scale EUV microscopy using a table-top laser source

High brightness Extreme Ultraviolet (EUV) sources for laboratory operation are needed in nano-fabrication and actinic (“at-wavelength”) inspection of the masks for high volume manufacturing in next generation lithography. Laser-plasma EUV sources have the required compactness and power scalability to achieve the demanding requirements. However, the incoherent emission lacks the brightness for single-shot high contrast imaging. On the other hand, fully coherent sources are considered to be unsuitable for full-field sample illumination and prone to speckles. We evaluate the capabilities of a lab-scale amplified-spontaneous-emission (ASE) EUV laser source to combine brightness and high quality imaging with full-field imaging, along with rapid acquisition and compactness.

Coulomb versus drag effects in a photoelectron bunch for extreme ultraviolet laser spectroscopy

Coulomb effects in an extreme ultraviolet laser-induced photoelectron bunch for spectroscopy were investigated computationally. Post-photoemission alteration of the trajectory, due to Coulombic interactions, hampers an accurate angle-resolved photoelectron spectroscopy. Simulations however demonstrated that operation in the redundant-population regime produces a drag-confined bunch, detached from a boundary sheath that experiences losses. Drastic reduction in the photoelectron density can loosen bunch-confinement and proportionally increase the boundary losses. Our simulations led to a critical number of photoelectrons per spot size equal to 1.5×104 e−/mm2.

Metallic-like droplets produced by irradiating rare-gas clusters with free electron laser pulses

Unlike metallic elements, rare-gas atoms remain non-metallic even if they are condensed. However, once rare-gas clusters are irradiated by extreme ultraviolet free electron laser (EUV-FEL) pulses with slightly higher energy than their ionization potential, they exhibit metallic-like behaviors because the ionization takes place sequentially within the clusters owing to the huge valence electron ionization cross section in the EUV regime. In this work Ar and Xe clusters were produced by pulsed supersonic jets, and the cluster beams were crossed synchronously with focused EUV-FEL beams ejected from the SCSS test accelerator in Japan. We measured time-of-flight (TOF) mass spectra and kinetic energy distribution (KED) of daughter ions produced via Coulomb explosion by using three dimensional (3D) momentum imaging spectrometer. The metallic-like nature is evidenced not only by widely spread charge distributions within the cluster but also by enhanced positive surface charges surrounded by quasi-free electron clouds.

Extreme ultraviolet interferometry of laser plasma material between the critical and ablation surfaces

Interferometric probing using an extreme ultraviolet (EUV) laser has measured both transmission and phase information through laser-irradiated plastic (parylene-N C 8H 8) targets (thickness 350 nm). Unusually, the probe beam is incident longitudinally in approximately the same direction as the incident optical laser. Agreement of the experimental interferometry results has been obtained with two-dimensional radiation hydrodynamic code (h2d) simulations of EUV (21.2 nm) probe transmissions and phase shifts. We show that the transmission of the EUV probe beam provides a measure of the rate of target ablation, as ablated plasma becomes close to transparent when the photon energy is less than the ionization energy of the predominate ion species. Here C 3+ ions with ionization energy 64.5 eV are transparent, while lower carbon ionization stages, present in the unablated target and close to the ablation surface, absorb the 58.5 eV photons. Similarly, we show that refractive indices η below the solid parylene-N ( η solid = 0.946) and expected plasma values are produced in the warm dense plasma created by laser irradiation due to bound–free absorption in C +.

Design of a phase shifting interferometer in the EUV for high precision metrology

We present the design of phase shift interferometer for the extreme ultraviolet (EUV) that will be used with the illumination provided by a table top Ne-like Ar laser emitting at 46.9 nm. We develop a model that computes the beam propagation trough the instrument, taking into account the influence of the fluctuations from shot-to-shot of the pulsed EUV laser on the retrieved wavefront.

Extreme ultraviolet free electron laser seeded with high-order harmonic of Ti:sapphire laser

The 13th harmonic of a Ti:sapphire (Ti:S) laser in the plateau region was injected as a seeding source to a 250-MeV free-electron-laser (FEL) amplifier. When the amplification conditions were fulfilled, strong enhancement of the radiation intensity by a factor of 650 was observed. The random and uncontrollable spikes, which appeared in the spectra of the Self-Amplified Spontaneous Emission (SASE) based FEL radiation without the seeding source, were found to be suppressed drastically to form to a narrow-band, single peak profile at 61.2 nm. The properties of the seeded FEL radiation were well reproduced by numerical simulations. We discuss the future precept of the seeded FEL scheme to the shorter wavelength region.

Multiple Ionization Bursts in Laser-Driven Hydrogen Molecular Ion

Theoretical study on H2(+) in an intense infrared laser field on the attosecond time scale reveals that the molecular ion shows multiple bursts of ionization within a half-cycle of the laser field oscillation, in contrast to the widely accepted tunnel ionization picture for an atom. These bursts are found to be induced by transient localization of the electron at one of the nuclei, and a relation between the time instants of the localization and the vector potential of the laser light is derived. A scheme is proposed to probe the localization dynamics by an extreme ultraviolet laser pulse.

Extreme ultraviolet interferometry of warm dense matter in laser plasmas

We demonstrate that interferometric probing with extreme ultraviolet (EUV) laser light enables determination of the degree of ionization of the "warm dense matter" produced between the critical and ablation surfaces of laser plasmas. Interferometry has been utilized to measure both transmission and phase information for an EUV laser beam at the photon energy of 58.5 eV, probing longitudinally through laser-irradiated plastic (parylene-N) targets (thickness 350 nm) irradiated by a 300 ps duration pulse of wavelength 438 nm and peak irradiance 10(12) W cm(-2). The transmission of the EUV probe beam provides a measure of the rate of target ablation, as ablated plasma becomes close to transparent when the photon energy is less than the ionization energy of the predominant ion species. We show that refractive indices η below the solid parylene N (η(solid) = 0.946) and expected plasma values are produced in the warm dense plasma created by laser irradiation due to bound-free absorption in C(+).

Experimental and theoretical studies of reactions of neutral vanadium and tantalum oxide clusters with NO and NH3

Reactions of neutral vanadium and tantalum oxide clusters with NO, NH(3), and an NO/NH(3) mixture in a fast flow reactor are investigated by time of flight mass spectrometry and density functional theory (DFT) calculations. Single photon ionization through a 46.9 nm (26.5 eV) extreme ultraviolet (EUV) laser is employed to detect both neutral cluster distributions and reaction products. Association products VO(3)NO and V(2)O(5)NO are detected for V(m)O(n) clusters reacting with pure NO, and reaction products, TaO(3,4)(NO)(1,2), Ta(2)O(5)NO, Ta(2)O(6)(NO)(1-3), and Ta(3)O(8)(NO)(1,2) are generated for Ta(m)O(n) clusters reacting with NO. In both instances, oxygen-rich clusters are the active metal oxide species for the reaction M(m)O(n)+NO→M(m)O(n)(NO)(x). Both V(m)O(n) and Ta(m)O(n) cluster systems are very active with NH(3). The main products of the reactions with NH(3) result from the adsorption of one or two NH(3) molecules on the respective clusters. A gas mixture of NO:NH(3) (9:1) is also added into the fast flow reactor: the V(m)O(n) cluster system forms stable, observable clusters with only NH(3) and no V(m)O(n)(NO)(x)(NH(3))(y) species are detected; the Ta(m)O(n) cluster system forms stable, observable mixed clusters, Ta(m)O(n)(NO)(x)(NH(3))(y), as well as Ta(m)O(n)(NO)(x) and Ta(m)O(n)(NH(3))(y) individual clusters, under similar conditions. The mechanisms for the reactions of neutral V(m)O(n) and Ta(m)O(n) clusters with NO/NH(3) are explored via DFT calculations. Ta(m)O(n) clusters form stable complexes based on the coadsorption of NO and NH(3). V(m)O(n) clusters form weakly bound complexes following the reaction pathway toward end products N(2)+H(2)O without barrier. The calculations give an interpretation of the experimental data that is consistent with the condensed phase reactivity of V(m)O(n) catalyst and suggest the formation of intermediates in the catalytic chemistry.

Ablative microstructuring with plasma-based XUV lasers and efficient processing of materials by dual action of XUV/NIR–VIS ultrashort pulses

We report on a single-shot micropatterning of an organic polymer achieved by ablation with demagnifying projection using a plasma-based extreme ultraviolet (XUV) laser at 21 nm. A nickel mesh with a period of 100 μ m was 10×demagnified and imprinted on poly(methyl methacrylate) (PMMA) via direct ablation. This first demonstration of single-shot projection, single-step lithography illustrates the great potential of XUV lasers for the direct patterning of materials with a resolution scalable down to the submicrometer domain. In the second part, we present a novel experimental method for improving the efficiency of surface processing of various solids achieved by simultaneous action of XUV, obtained from high-order harmonic generation, and near-infrared (NIR)–VIS laser pulses. The NIR–VIS pulse interacts with free charge carriers produced by the energetic XUV photons, so that its absorption dramatically increases. Laser-induced periodic surface structures were effectively produced using this technique.

Multiphoton Double Ionization of Ar in Intense Extreme Ultraviolet Laser Fields Studied by Shot-by-Shot Photoelectron Spectroscopy

Photoelectron spectroscopy has been performed to study the multiphoton double ionization of Ar in an intense extreme ultraviolet laser field (hν ∼ 21 eV, ∼ 5 TW/cm²), by using a free electron laser (FEL). Three distinct peaks identified in the observed photoelectron spectra clearly show that the double ionization proceeds sequentially via the formation of Ar(+): Ar+hν→Ar (+) + e⁻ and Ar²(+) + 2hν→Ar(+) + e⁻. Shot-by-shot recording of the photoelectron spectra allows simultaneous monitoring of FEL spectrum and the multiphoton process for each FEL pulse, revealing that the two-photon ionization from Ar(+) is significantly enhanced by intermediate resonances in Ar(+).

Measurement of the single-shot pulse energy of a free electron laser using a cryogenic radiometer

The absolute single-shot pulse energy of the SPring 8 extreme ultraviolet (EUV) free electron laser (FEL) was measured using a cryogenic radiometer with a relative standard uncertainty of 3%. The temperature change of the cavity in the cryogenic radiometer caused by an incident FEL pulse was determined using a lock-in amplifier and an ac Wheatstone bridge. The measured pulse energies were compared with a gas-monitor detector developed by Physikalisch-Technische Bundesanstalt/Deutsches Elektronen-Synchrotron/Ioffe Physico-Technical Institute (Ioffe) at a wavelength of 51.3 nm at the SPring-8 EUV-FEL in a shot-to-shot mode. The pulse energies measured using the two detectors agree within 2.0%.

Ionization heating in rare-gas clusters under intense XUV laser pulses

The interaction of intense extreme ultraviolet (XUV) laser pulses ($\ensuremath{\lambda}=32 \mathrm{nm}$, $I={10}^{11}--{10}^{14}$ W/cm${}^{2}$) with small rare-gas clusters (${\mathrm{Ar}}_{147}$) is studied by quasiclassical molecular dynamics simulations. Our analysis supports a very general picture of the charging and heating dynamics in finite samples under short-wavelength radiation that is of relevance for several applications of free-electron lasers. First, up to a certain photon flux, ionization proceeds as a series of direct photoemission events producing a jellium-like cluster potential and a characteristic plateau in the photoelectron spectrum as observed in Bostedt et al. [Phys. Rev. Lett. 100, 133401 (2008)]. Second, beyond the onset of photoelectron trapping, nanoplasma formation leads to evaporative electron emission with a characteristic thermal tail in the electron spectrum. A detailed analysis of this transition is presented. Third, in contrast to the behavior in the infrared or low vacuum ultraviolet range, the nanoplasma energy capture proceeds via ionization heating, i.e., inner photoionization of localized electrons, whereas collisional heating of conduction electrons is negligible up to high laser intensities. A direct consequence of the latter is a surprising evolution of the mean energy of emitted electrons as function of laser intensity.

Ion-ion coincidence studies on multiple ionizations of N2 and O2 molecules irradiated by extreme ultraviolet free-electron laser pulses

We have investigated multiple ionization of N(2) and O(2) molecules by 52 nm extreme-ultraviolet light pulses at the free-electron laser facility SCSS in Japan. Coulomb break-up of parent ions with charge states up to 5+ is found by the ion-ion coincidence technique. The charge-state dependence of kinetic energy release distributions suggests that the electrons are emitted sequentially in competition with the elongation of the bond length.

A study of the mechanical vibrations of a table-top extreme ultraviolet interference nanolithography tool

A prototype low cost table-top extreme ultraviolet (EUV) laser source (1.5 ns pulse duration, lambda=46.9 nm) was successfully employed as a laboratory scale interference nanolithography (INL) tool. Interference patterns were obtained with a simple Lloyd's mirror setup. Periodic structures on Polymethylmethacrylate/Si substrates were produced on large areas (8 mm(2)) with resolutions from 400 to 22.5 nm half pitch (the smallest resolution achieved so far with table-top EUV laser sources). The mechanical vibrations affecting both the laser source and Lloyd's setup were studied to determine if and how they affect the lateral resolution of the lithographic system. The vibration dynamics was described by a statistical model based on the assumption that the instantaneous position of the vibrating mechanical parts follows a normal distribution. An algorithm was developed to simulate the process of sample irradiation under different vibrations. The comparison between simulations and experiments allowed to estimate the characteristic amplitude of vibrations that was deduced to be lower than 50 nm. The same algorithm was used to reproduce the expected pattern profiles in the lambda/4 half pitch physical resolution limit. In that limit, a nonzero pattern modulation amplitude was obtained from the simulations, comparable to the peak-to-valley height (2-3 nm) measured for the 45 nm spaced fringes, indicating that the mechanical vibrations affecting the INL tool do not represent a limit in scaling down the resolution.