Extreme Ultraviolet Light Research Articles

Microdroplet-tin plasma sources of EUV radiation driven by solid-state-lasers (Topical Review)

Plasma produced from molten-tin microdroplets generates extreme ultraviolet light for state-of-the-art nanolithography. Currently, CO2 lasers are used to drive the plasma. In the future, solid-state mid-infrared lasers may instead be used to efficiently pump the plasma. Such laser systems have promise to be more compact, better scalable, and have higher wall-plug efficiency. In this Topical Review, we present recent findings made at the Advanced Research Center for Nanolithography (ARCNL) on using 1 and 2 µm wavelength solid-state lasers for tin target preparation and for driving hot and dense plasma. The ARCNL research ranges from advanced laser development, studies of fluid dynamic response of droplets to impact, radiation-hydrodynamics calculations of, e.g. ion ‘debris’, (EUV) spectroscopic studies of tin laser-produced-plasma as well as high-conversion efficiency operation of 2 µm wavelength driven plasma.

Photonic crystal L3 cavity laser fabricated using maskless digital photolithography

Abstract Projection photolithography using an extreme-ultraviolet light source is the core technology that has enabled patterning on the scale of a few nanometers that is required for modern electronic chips. However, this high-end system is neither affordable nor needed for photonics where critical feature sizes are of 100s of nanometers (or of submicron). Although electron-beam lithography can provide a means for photonic device fabrication, it suffers from extremely low throughput. Therefore, a lithographic technique for submicron pattern generation at high throughput and low cost is in high demand. This group recently showed that maskless digital photolithography (MDPL), a convenient and versatile photolithographic technique that requires no photomask, could potentially address this demand by demonstrating photonic crystal (PhC) patterns with submicron periodicity and associated PhC band-edge lasers. In this paper, we report the fabrication of a PhC L3 cavity laser, which contains irregular air holes in terms of their positions and sizes, using the MDPL technique. Successful generation of such an aperiodic and nontrivial submicron pattern requires thorough understanding and scrupulous manipulation on light diffraction. Our achievements should provide the concrete foundation upon which compact, versatile, convenient, speedy, and economical lithographic tools for arbitrary submicron pattern generation can be developed.

Valence Band of Rutile TiO2(110) Investigated by Polarized-Light-Based Angle-Resolved Photoelectron Spectroscopy.

Band structure dictates optical and electronic properties of solids and eventually the efficiency of the semiconductor based solar conversion. Compared to numerous theoretical calculations, the experimentally measured band structure of rutile TiO2, a prototypical photocatalytic material, is rare. In this work, the valence band structure of rutile TiO2(110) is measured by angle-resolved photoelectron spectroscopy using polarized extreme ultraviolet light. The effective mass of the hole, which has never been measured before, is determined to be 4.66-6.87 m0 (free electron mass) and anisotropic. The dependence of photoemission intensities on excitation light polarization is analyzed by taking into account of the parity symmetry of molecular orbitals in the blocking unit of rutile TiO2. This work reports a direct measurement of valence band structure and hole effective mass of rutile TiO2(110), which will deepen our understanding of the electronic structure and charge carrier properties of the model material and provide reference data for future theoretical calculations.

A narrow bandwidth extreme ultra-violet light source for time- and angle-resolved photoemission spectroscopy.

Here, we present a high repetition rate, narrow bandwidth, extreme ultraviolet photon source for time- and angle-resolved photoemission spectroscopy. The narrow bandwidth pulses meV for photon energies eV are generated through high harmonic generation using ultra-violet drive pulses with relatively long pulse lengths (461 fs). The high harmonic generation setup employs an annular drive beam in tight focusing geometry at a repetition rate of 250 kHz. Photon energy selection is provided by a series of selectable multilayer bandpass mirrors and thin film filters, thus avoiding any time broadening introduced by single grating monochromators. A two stage optical-parametric amplifier provides < 100 fs tunable pump pulses from 0.65 μm to 9 μm. The narrow bandwidth performance of the light source is demonstrated through angle-resolved photoemission measurements on a series of quantum materials, including high-temperature superconductor Bi-2212, WSe2, and graphene.

Macroscopic phase-matching mechanism for orbital angular momentum spectra of high-order harmonics by mixing two Laguerre-Gaussian vortex modes

The high-order harmonic generation (HHG) by the interaction of an intense vortex infrared laser and a gas medium has been employed to produce the extreme ultraviolet (XUV) light beam carrying a high value orbital angular momentum (OAM). Here we extend this approach to generate the XUV light with superimposed OAM modes by mixing two different Laguerre-Gaussian (LG) modes as the driving beam. By solving the three-dimensional Maxwell's wave equations of the high-harmonic field and calculating the coherence lengths of HHG, we reveal the complex nature of phase-matching conditions in the gas medium, especially their dependence on the azimuthal angle. We demonstrate that the OAM spectra of the HHG can be tailored by varying the harmonic order, the position of gas medium, and the energy ratio of two LG beams. We also uncover that only including short-trajectory contribution in the single-atom response could broaden the OAM spectrum of the macroscopic HHG because of the featured phase-matching characteristics caused by the atomic intrinsic phase. We anticipate this work to stimulate some interests in generating an XUV vortex beam with the tunable OAM spectrum through the gaseous HHG process as well as in separating different OAM modes of an XUV vortex beam by advanced techniques.

Modeling the wavelength of unresolved transition arrays in the extreme ultraviolet region from Sn to Hf ions by combining theoretical and experimental spectral data

This paper proposes a method to determine the wavelength of unresolved transition arrays (UTAs) in the extreme ultraviolet (EUV) wavelength region from Sn to Hf plasma by combining calculated and experimental data. Based on a computational analysis of the atomic structure, we show that the wavelength of UTAs can be explained using the screening theory by a simple quadratic formula using the effective core charge and the screening constant for 4d electrons as parameters. The results from the model were compared with experiments to reproduce the trend of the spectrum, which has a minimum wavelength with respect to the ion charge. The wavelength is shown to agree with experiment over Pd- to Sr-like ions by applying a small shift that was determined using the spectrum observed in the electron beam ion trap. The present model would allow us to calculate the opacity of Sn plasmas with much smaller computational time than using present large-scale collisional radiative models, with fewer energy levels and parameterized rate coefficients, which will be also useful to investigate the efficiency of the EUV light source.

Organic abrasive machining system for optical fabrication with 0.1-mm spatial resolution.

High-precision optics for short-wavelength regions, such as x rays and extreme ultraviolet light, generally require nanometer-level figure accuracy on their surfaces. Such optics are finished via a numerically controlled figure correction process in which the dwelling time of the machining tool on the workpiece is controlled. Due to the limitation of the machined spot size, it is difficult to remove mid-spatial-frequency (1 to 10mm-1) errors on an optical surface. To realize a high-spatial-resolution figure correction process for high-precision optics, we have been developing the organic abrasive machining (OAM) technique, which can generate a 100 µm machined spot using a small elastic rotation tool in a slurry that includes acrylic particles. In this study, an OAM apparatus that can measure the machining load was constructed. The effects of the machining and slurry conditions were investigated and high-spatial-resolution machining on a flat glass substrate was demonstrated. The root-mean-square roughness of the surface after OAM processing was below 0.2nm. Patterns with a minimum line and space size of 100 µm were successfully fabricated.

Line-shape broadening of an autoionizing state in helium at high XUV intensity

We study the interaction of intense extreme ultraviolet (XUV) light with the 2s2p doubly excited state in helium. In addition to previously understood energy-level and phase shifts, high XUV intensities may lead to other absorption-line-shape distortions. Here, we report on experimental transient-absorption spectroscopy results on the 2s2p line-width modification in helium in intense stochastic XUV fields. A few-level-model simulation is realized to investigate the origins of this effect. We find that the line-shape broadening is connected to the strong coupling of the ground state to the 2s2p doubly excited state which is embedded in the ionization continuum. As the broadening takes place for intensities lower than for other strong-coupling processes, e.g. observed asymmetry changes of the absorption profile, this signature can be identified already in an intermediate intensity regime. These findings are in general relevant for resonant inner-shell transitions in nonlinear experiments with XUV and x-ray photon energies at high intensity.

Investigation of correlative parameters to evaluate EUV lithographic performance of PMMA.

Investigations to evaluate the extreme ultraviolet (EUV) lithographic performance of 160 nm thick poly(methyl methacrylate) with 13.5 nm wavelength EUV light were performed using a synchrotron radiation source at Pohang Light Source-II (PLS-II). The single system enabled the determination of the sensitivity, contrast, linear absorption coefficient, critical dimension, and line edge roughness of polymer thin films through tests and measurements. The experimental findings were also compared to theoretical results and those of previously reported studies. According to the results of the dose-to-clear test and transmission measurements, the critical dimension of a line and space pattern (>50 nm) via interference lithography with 250 nm pitch grating agreed well with the results calculated using the lumped parameter model. The experimental results demonstrated that the equipment and test protocol can be used for EUV material infrastructure evaluation in academia and in industry.

Generation, manipulation, and application of high-order harmonics in solids

The generation of high-order harmonics based on the interaction between ultrafast intense laser and matter provides a platform for studying the light-matter interaction in the non-perturbative region. It is also the main route to generating desktop extreme ultraviolet light source and attosecond pulse. The non-perturbative solid high-order harmonic involves the core content of ultrafast strong field physics, condensed matter physics, materials science, information science and other fields. Since it was first experimentally observed in 2011, it has rapidly become the research frontier of strong field physics and attosecond science. This review summarizes the research progress and important applications of solid high-order harmonics from the perspective of an experimentalist. Firstly, distinct characteristics are shown for solid high-order harmonic by comparing the dependence of harmonic yield and cut-off energy on driving laser parameters with gas high-order harmonic. Then, the progress of manipulation and application are highlighted for solid high-order harmonic, including the precise control of harmonic yield, polarization, space-time distribution through the design of target structure or laser field, as well as the application of solid high-order harmonic spectroscopy in the fields of material structure characterization and ultrafast electron dynamics. Finally, the future is prospected for the study of solid high-order harmonics.

Optimizing high harmonic generation in hollow-core gas cell considering variation of gas density

We have developed a coherent and compact extreme-ultraviolet light source based on phase-matched high harmonic generation by using a hollow-core gas cell that can be easily aligned and maintain long stability. The gas cell consists of three bodies to minimize gas leakage and maintain stable vacuum. The photon flux was calculated considering the dependence of the gas number density and the pressure on the radii of the hollow core and the hole in the Al plates on both sides of the gas cell, which showed good coincidence with the experimental values.The photon flux is 2 × 1010 photons s−1 near 13.5 nm (91.5 eV) within 10 nm bandwidth. Also, the compact extreme-ultraviolet light source is found to operate stably for hours, which is suitable for practical applications such as metrology and inspection for extreme-ultraviolet mask, spectroscopy, holography, microscopy, etc.

The spectrum of a 1- μ m-wavelength-driven tin microdroplet laser-produced plasma source in the 5.5–265.5 nm wavelength range

We present a calibrated spectrum in the 5.5–265.5 nm range from a microdroplet-tin Nd:YAG-laser-produced plasma under conditions relevant for the production of extreme ultraviolet (EUV) light at 13.5 nm for nanolithography. The plasma emission spectrum obtained using a custom-built transmission grating spectrometer results from a careful calibration of a series of filters enabling measurements free of any higher diffraction orders. Specifically, Zr, Si, and Al thin-foil filters and bulk LiF, MgF2, and UV fused silica filters are employed. A further filter using four SiC mirrors is used to record the otherwise inaccessible 40–100 nm range. The resulting corrected and concatenated spectra are shown to accurately match in their respective overlap regions. The possibility to measure spectra over this broad range enables the optimization of current and future sources of EUV light for nanolithography by providing the diagnostics required for minimizing the emission of unwanted wavelength bands.

Electron quantum path control in high harmonic generation via chirp variation of strong laser pulses

The quantum phases of the electron paths driven by an ultrafast laser in high harmonic generation in an atomic gas depends linearly on the instantaneous cycle-averaged laser intensity. Using high laser intensities, a complete single ionisation of the atomic gas may occur before the laser pulse peak. Therefore, high harmonic generation could be localised only in a temporal window at the leading edge of laser pulse envelope. Varying the laser frequency chirp of an intense ultrafast laser pulse, the centre, and the width of the temporal window, that the high harmonic generation phenomenon occurs, could be controlled with high accuracy. This way, both the duration and the phase of the electron trajectories, that generate efficiently high harmonics, is fully controlled. A method of spectral control and selection of the high harmonic extreme ultraviolet light from distinct quantum paths is experimentally demonstrated. Furthermore, a phenomenological numerical model enlightens the physical processes that take place. This novel approach of the electron quantum path selection via laser chirp is a simple and versatile way of controlling the time-spectral characteristics of the coherent extreme ultraviolet light with applications in the fields of attosecond pulses and soft x-ray nano-imaging.

XUV-Initiated Dissociation Dynamics of Molecular Oxygen (O2)

We performed a time-resolved spectroscopy experiment on the dissociation of oxygen molecules after the interaction with intense extreme-ultraviolet (XUV) light from the free-electron laser in Hamburg at Deutsches Elektronen-Synchrotron. Using an XUV-pump/XUV-probe transient-absorption geometry with a split-and-delay unit, we observe the onset of electronic transitions in the O2+ cation near 50 eV photon energy, marking the end of the progression from a molecule to two isolated atoms. We observe two different time scales of 290 ± 53 and 180 ± 76 fs for the emergence of different ionic transitions, indicating different dissociation pathways taken by the departing oxygen atoms. With regard to the emerging opportunities of tuning the central frequencies of pump and probe pulses and of increasing the probe–pulse bandwidth, future pump–probe transient-absorption experiments are expected to provide a detailed view of the coupled nuclear and electronic dynamics during molecular dissociation.

Diffraction-limited coherent wake emission

The plasma mirror is a relativistic optical element that under certain irradiation conditions generates intense attosecond extreme-ultraviolet light pulses, in a process known as coherent wake emission (CWE). CWE has been previously characterized by its high spatial divergence, originating from an intrinsic intensity-dependent phase accumulation. In this Letter, we show that the transverse variations of the plasma expansion can completely cancel the CWE intrinsic phase. Accordingly, we experimentally demonstrate nearly diffraction-limited CWE with unprecedented divergence, under 6 mrad. We validate our analytical model with particle in cell simulations. This understanding facilitates the development of plasma mirrors as applicable ultraviolet light sources.Received 9 March 2021Accepted 5 August 2021DOI:https://doi.org/10.1103/PhysRevResearch.3.L032059Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasHigh intensity laser-plasma interactionsHigh-order harmonic generationPhysical SystemsRelativistic plasmasAtomic, Molecular & OpticalPlasma Physics

Bottom-Up Nanofabrication with Extreme-Ultraviolet Light: Metal-Organic Frameworks on Patterned Monolayers.

The fabrication of integrated circuits with ever smaller (sub-10 nm) features poses fundamental challenges in chemistry and materials science. As smaller nanostructures are fabricated, thinner layers of materials are required, and surfaces and interfaces gain a more important role in the formation of nanopatterns. We present a new bottom-up approach in which we use the high optical resolution offered by extreme ultraviolet (EUV) lithography to print patterns on self-assembled monolayers (SAMs). Upon radiation, low-energy electrons induce chemical changes in the SAM so that the projected image is transferred to the substrate surface. We use the chemical differences between exposed and unexposed regions to promote a selective growth of hybrid structures that can act as an etch-resistant layer for further pattern transfer or can be used as functional nanostructures. The EUV doses required to promote selective growth on exposed areas are close to industrial requirements. Furthermore, this method allows for the independent tuning of different steps in the EUV lithography process (photo-induced chemistry, spatially resolved chemical contrast, and formation of nanopatterns), an advantage over current resists, in which the same material plays all roles.

Intense quasi-monochromatic resonant harmonic generation in the multiphoton ionization regime

Resonant high-order harmonics, which result in quasi-monochromatic extreme ultraviolet light with coherent intensity enhancement involving autoionizing resonances, have been demonstrated from laser-ablated plumes in the tunnel-ionization regime. Here, we demonstrate resonant harmonics in the previously unexplored multiphoton-ionization regime. We demonstrate an intense resonant harmonic from gallium with an intensity enhancement ratio of 714 relative to the neighboring harmonics, achieved without the need for extreme ultraviolet filtering methods, thus preventing a typical photon flux loss of more than 70%. Three-dimensional time-dependent Schrödinger equation calculations reveal that this increase in the enhancement ratio is due to the low electron wave packet spreading in the multiphoton-ionization regime. These results reveal a method for increasing the intensity and monochromaticity of intense multimicrojoule femtosecond extreme ultraviolet light and will also facilitate understanding of the involvement of autoionizing resonances in generating resonant harmonics in the multiphoton-ionization regime.

Agile spectral tuning of high order harmonics by interference of two driving pulses.

In this work, the experimental realization of a tunable high photon flux extreme ultraviolet light source is presented. This is enabled by high harmonic generation of two temporally delayed driving pulses with a wavelength of 1030 nm, resulting in a tuning range of 0.8 eV at the 19th harmonic at 22.8 eV. The implemented approach allows for fast tuning of the spectrum, is highly flexible and is scalable towards full spectral coverage at higher photon energies.

Characterization of angularly resolved EUV emission from 2-µm-wavelength laser-driven Sn plasmas using preformed liquid disk targets

The emission properties of tin plasmas, produced by the irradiation of preformed liquid tin targets by several-ns-long 2 µm-wavelength laser pulses, are studied in the extreme ultraviolet (EUV) regime. In a two-pulse scheme, a pre-pulse laser is first used to deform tin microdroplets into thin, extended disks before the main (2 µm) pulse creates the EUV-emitting plasma. Irradiating 30- to 300 µm-diameter targets with 2 µm laser pulses, we find that the efficiency in creating EUV light around 13.5 nm follows the fraction of laser light that overlaps with the target. Next, the effects of a change in 2 µm drive laser intensity (0.6–1.8 × 1011 W cm−2) and pulse duration (3.7–7.4 ns) are studied. It is found that the angular dependence of the emission of light within a 2% bandwidth around 13.5 nm and within the backward 2π hemisphere around the incoming laser beam is almost independent of intensity and duration of the 2 µm drive laser. With increasing target diameter, the emission in this 2% bandwidth becomes increasingly anisotropic, with a greater fraction of light being emitted into the hemisphere of the incoming laser beam. For direct comparison, a similar set of experiments is performed with a 1 µm-wavelength drive laser. Emission spectra, recorded in a 5.5–25.5 nm wavelength range, show significant self-absorption of light around 13.5 nm in the 1 µm case, while in the 2 µm case only an opacity-related broadening of the spectral feature at 13.5 nm is observed. This work demonstrates the enhanced capabilities and performance of 2 µm-driven plasmas produced from disk targets when compared to 1 µm-driven plasmas, providing strong motivation for the use of 2 µm lasers as drive lasers in future high-power sources of EUV light.

Controlling quantum numbers and light emission of Rydberg states via the laser pulse duration

High Harmonic Generation (HHG) creates coherent high frequency radiation via the process of strong field ionization followed by recombination. Recently, a complementary approach based on Frustrated Tunnel Ionization (FTI) was demonstrated (Nature Photonics 12, 620 (2018)). It uses spectrally separated peaks created by lower quantum number Rydberg states to produce coherent extreme ultraviolet (EUV) light. While much is understood about enhancing emission from HHG by controlling recombining electron trajectories, relatively little is known about controlling the quantum number distribution of Rydberg states. This distribution is generally believed to be determined primarily by field strength and laser frequency. We show that, in fact, it also changes significantly with the duration of the laser pulse: increasing pulse duration depletes lower-lying Rydberg states, thereby substantially decreasing EUV yield. Using electron trajectory analysis, we identify elastic recollision as the underlying cause. Our results open a door to greater control over production of coherent high frequency radiation, by combining FTI and HHG mechanisms, and also improved the interpretation of molecular imaging experiments that rely on elastic electron recollision.