This PDF file contains the front matter associated with SPIE Proceedings Volume 10243, including the Title Page, Copyright information, Table of Contents, Introduction (if any), and Conference Committee listing.

We report here recent work on an optical-field ionized (OFI), high-order harmonic-seeded EUV laser. The amplifying medium is a plasma of nickel-like krypton obtained by optical field ionization focusing a 1 J, 30 fs, circularly- polarized, infrared pulse into a krypton-filled gas cell or krypton gas jet. The lasing transition is the 3d94p (J=0) −→ 3d94p (J=1) transition of Ni-like krypton ions at 32.8 nm and is pumped by collisions with hot electrons. The polarization of the HH-seeded EUV laser beam was studied using an analyzer composed of three grazing incidence EUV multilayer mirrors able to spin under vacuum. For linear polarization, the Malus law has been recovered while in the case of a circularly-polarized seed, the EUV signal is insensitive to the rotation of the analyzer, bearing testimony to circularly polarized. The gain dynamics was probed by seeding the amplifier with a high-order harmonic pulse at different delays. The gain duration monotonically decreased from 7 ps to an unprecedented shortness of 450 fs FWHM as the amplification peak rose from 150 to 1,200 with an increase of the plasma density from 3 × 1018 cm−3 up to 1.2 × 1020 cm−3. The integrated energy of the EUV laser pulse was also measured, and found to be around 2 μJ. It is to be noted that in the ASE mode, longer amplifiers were achieved (up to 3 cm), yielding EUV outputs up to 14 μJ.

The amplification of UV radiation and high order harmonics (HOH) in plasmas is a subject of raising interest due to its different potential applications in several fields like environment and security (detection at distance), biology, materials science and industry (3D imaging) and atomic and plasma physics (pump-probe experiments). In order to develop these sources, it is necessary to properly understand the amplification process. Being the plasma an inhomogeneous medium which changes with time, it is desirable to have a full time-dependent 3D description of the interaction of UV and XUV radiation with plasmas. For these reasons, at the Instituto de Fusi´on Nuclear we have developed DAGON, a 3D Maxwell-Bloch code capable of studying the full spationtemporal structure of the amplification process abovementioned.

It was medical applications that stimulated F. Carrol in the early 1990s to start the research of on relativistic Thomson scattering X-ray sources, as a part of the infrastructure of the future society. The possibility to use such a source in interventional cardiology is discussed in this paper. The replacement of X-ray tube by relativistic Thomson scattering Xray source is predicted to lower the patient radiation dose by a factor of 3 while image quality remains the same. The required general characteristics of accelerator and laser units are found. They can be reached by existing technology. A semiempirical method for simulation of medical and technical parameters of interventional coronary angiography systems is suggested.

Near edge X-ray absorption fine structure (NEXAFS) spectroscopy in the soft X-ray range is feasible in the laboratory using laser-produced plasma sources. We present a study using seven different target materials for optimized data analysis. The emission spectra of the materials with atomic numbers ranging from Z = 6 to Z = 79 show distinct differences, rendering the adapted selection of a suitable target material for specialized experiments feasible. For NEXAFS spectroscopy a 112.5 nm thick polyimide film is investigated as a reference exemplifying the superiority of quasi-continuum like emission spectra.

In this contribution, we report about nanoscale imaging using a laser produced plasma source based laboratory transmission X-ray microscope (LTXM) in the water window. The highly brilliant soft X-ray radiation of the LTXM is provided by a laser-produced nitrogen plasma source focused by a multilayer condenser mirror to the sample. An objective zone plate maps the magnified image of the sample on the super resolution camera. This camera employs a deep cooled soft-X-ray CCD imaging sensor sandwiched with a xy piezo stage to allow subpixel displacements of the detector. The camera is read out using a very low noise electronics platform, also directing low µm shifts of the sensor between subsequent image acquisitions. Finally an algorithm computes a high resolution image from the individual shifted low-resolution image frames.

Short-pulse x-ray/gamma-ray sources have become indispensable light sources for investigating material science, bio technology, and photo-nuclear physics. In past decades, rapid advancement of high intensity laser technology led extensive progresses in the field of radiation sources based on laser-plasma interactions - x-ray lasers, betatron radiation and Compton gamma-rays. Ever since the installation of a 100-TW laser in 2006, we have pursued the development of ultrashort x-ray/gamma-ray radiations, such as x-ray lasers, relativistic high-order harmonics, betatron radiation and all-optical Compton gamma-rays. With the construction of two PW Ti:Sapphire laser beamlines having peak powers of 1.0 PW and 1.5 PW in 2010 and 2012, respectively [1], we have investigated the generation of multi-GeV electron beams [2] and MeV betatron radiations. We plan to carry out the Compton backscattering to generate MeV gamma-rays from the interaction of a GeV electron beam and a PW laser beam. Here, we present the recent progress in the development of ultrashort x-ray/gamma-ray radiation sources based on laser plasma interactions and the plan for developing Compton gamma-ray sources driven by the PW lasers. In addition, we will present the applications of laser-plasma x-ray lasers to x-ray holography and coherent diffraction imaging. [references] 1. J. H. Sung, S. K. Lee, T. J. Yu, T. M. Jeong, and J. Lee, Opt. Lett. 35, 3021 (2010). 2. H. T. Kim, K. H. Pae, H. J. Cha, I J. Kim, T. J. Yu, J. H. Sung, S. K. Lee, T. M. Jeong, J. Lee, Phys. Rev. Lett. 111, 165002 (2013).

Six years ago an inner-shell X-ray laser was demonstrated at 849 eV in singly ionized neon using the X-FEL at 960 eV to photo-ionize the 1s electron in neutral neon followed by lasing on the 2p – 1s transition in singly-ionized neon. It required a very strong X-ray source that could photo-ionize the 1s (K-shell) electron on a time scale comparable to the intrinsic auger lifetime of 2 fsec. We extend this work from K-shell to L-shell transitions. We show how the XFEL could be used photo-ionize L-shell electrons to drive gain on n=3-2 transitions in singly-ionized Ar and Cu plasmas. For Ar this requires an XFEL above 250 or 330 eV with lasing on 3-2 lines at 220 and 310 eV. The Cu scheme requires an XFEL above 960 eV with lasing on 3d-2p lines at 928 and 948 eV. We will also discuss extending this work to photoionizing the M-shell with lasing on n=4-3 transitions in singly ionized neodymium.

Stimulated emission is a fundamental process in nature that deserves to be investigated and understood in the EUV and X-ray regimes. Today this is definitely possible through high energy density FEL beams. In this context, we show evidence for soft x-ray stimulated emission from a MgO solid target pumped by extreme ultraviolet FEL pulses formed in the regime of travelling-wave amplified spontaneous emission in backward geometry. Our results combine two effects separately reported in previous works: emission in a privileged direction and existence of a material-dependent threshold, for the stimulated emission. We have developed a theoretical framework, based on coupled rate and transport equations taking into account the solid density plasma state of the target. Our model, accounts for both observed mechanisms that are the privileged direction for the stimulated emission of the Mg L_2,3 characteristic emission and the pumping threshold.

We will review recent progress in the development of high repetition, high average power rate soft x-ray lasers at 10-20 nm wavelength at Colorado State University, and the compact diode- pumped solid state lasers that drive them. The latter includes the development of a 1 J picosecond laser capable of operating at 500 Hz repetition rate. Results that demonstrate soft x-ray laser operation at the highest repetition rate reported to date: 400 Hz, and prospects of the use of these lasers in applications are discussed.

We have previously shown soft x-ray laser ablation time-of-flight mass spectrometry has the ability to detect singly ionized alanine molecules arising from the single shot ablation of a ∼50 zeptoliter volume. This superior sensitivity results from the ability to focus the 46.9 nm wavelength (26.4 eV energy per photon) laser beam to the diffraction limit, the strong absorption, and the efficient photoionization of the soft x-ray photons. In this paper we describe results on the application of soft x-ray laser mass spectrometry to elemental trace analysis in inorganic materials. Two dimensional imaging with spatial resolution of 80 nm in inorganic samples is also demonstrated.

Two-color laser pulses in a laboratory setup are interesting for enabling a number of advanced spectroscopy techniques. The generation by means of Ni-like laser-produced plasmas is promising for scaling down the wavelength towards the soft X-ray. The occurrence of a two-color signal has been documented in the 1990s and a detailed atomic physics study interpreted the pulse as due to concomitant collisional pumping (color-1) and self-photoexcitation (color-2). If this framework is on the atomic physics basis valid, its kinetic and hydrodynamic quantitative aspects need to be better understood. In particular, experimental observations leave room for a number of open points. Here we propose am amplified Raman scattering (ARS) scheme, to explain the growth of color-2 and its sensitivity to the plasma irradiation scheme.

Betatron x-ray radiation, driven by electrons from laser-wakefield acceleration, has unique properties to probe high energy density (HED) plasmas and warm dense matter. Betatron radiation is produced when relativistic electrons oscillate in the plasma wake of a laser pulse. Its properties are similar to those of synchrotron radiation, with a 1000 fold shorter pulse. This presentation will focus on the experimental challenges and results related to the development of betatron radiation for x-ray absorption spectroscopy of HED matter at large-scale laser facilities. A detailed presentation of the source mechanisms and characteristics in the blowout regime of laser-wakefield acceleration will be followed by a description of recent experiments performed at the Linac Coherent Light Source (LCLS). At LCLS, we have recently commissioned the betatron x-ray source driven by the MEC short pulse laser (1 J, 40 fs). The source is used as a probe for investigating the X-ray absorption near edge structure (XANES) spectrum at the K- or L-edge of iron and silicon oxide driven to a warm dense matter state (temperature of a few eV and solid densities). The driver is either LCLS itself or an optical laser. These experiments demonstrate the capability to study the electron-ion equilibration mechanisms in warm dense matter with sub-picosecond resolution.

X-ray-pump/x-ray-probe spectroscopy allows investigation of ultrafast x-ray induced molecular dynamics. X-ray absorption and Auger decay leave molecules in manifolds of transient intermediate states in the femtosecond time scale. By using an x-ray probe pulse, we can image nuclear wavepackets as a function of time using ion-ion coincidence spectroscopy to record ion momentum distributions and kinetic energy releases (KERs). Numerical simulations, a timedependent approach that includes both K-shell photoionization and Auger decay, show how the transient intermediate states are projected onto the KERs. At short time delays, the measurements are sensitive to interatomic interactions, whereas at longer delays the contribution from separated ions due to dissociative intermediate states becomes observable. We present simulations for the nitrogen molecule. These simulations have the potential to be extended to more complex molecules.

Among the fourth-generation light sources, the Italian free-electron laser (FEL) FERMI is the only one operating in the high-gain harmonic generation (HGHG) seeding mode. FERMI delivers pulses characterized by a quasi transform limited temporal structure, photon energies lying in the extreme ultra-violet (EUV) region, supreme transversal and longitudinal coherences, high peak brilliance, and full control of the polarization. Such state of the art performances recently opened the doors to a new class of time-resolved spectroscopies, difficult or even impossible to be performed using self-amplified spontaneous sources (SASE) light sources. FERMI is currently equipped with three operating beamlines opened to external users (DiProI, LDM and EIS), while two more are under commissioning (MagneDYN and TeraFERMI). Here, we present the recent highlights of the EIS (Elastic and Inelastic Scattering) beamline, which has been purposely designed to take full advantage from the coherence, the intensity, the harmonics content, and the temporal duration of the pulses. EIS is a flexible experimental facility for time-resolved EUV scattering experiments on condensed matter systems, consisting of two independent end-stations. The first one (EIS-TIMEX) aims to study materials in metastable and warm dense matter (WDM) conditions, while the second end-station (EIS-TIMER) is fully oriented to the extension of four-wave mixing (FWM) spectroscopies towards the EUV spectral regions, trying to reveal the behavior of matter in portions of the mesoscopic regime of exchanged momentum impossible to be probed using conventional light sources.

In this work we present experimental, compact desk-top SXR microscope, the EUV microscope which is at this stage a technology demonstrator, and finally, the SXR contact microscope. The systems are based on laser-plasma EUV and SXR sources, employing a double stream gas puff target. The EUV and SXR full field microscopes, operating at 13.8 nm and 2.88 nm wavelengths, respectively, are capable of imaging nanostructures with a sub-50 nm spatial resolution with relatively short (seconds) exposure times. The SXR contact microscope operates in the “water-window” spectral range, to produce an imprint of the internal structure of the sample in a thin layer of SXR light sensitive photoresist. Applications of such desk-top EUV and SXR microscopes for studies of variety of different samples – test objects for resolution assessment and other objects such as carbon membranes, DNA plasmid samples, organic and inorganic thin layers, diatoms, algae and carcinoma cells, are also presented. Details about the sources, the microscopes as well as the imaging results for various objects will be presented and discussed. The development of such compact imaging systems may be important to the new research related to biological, material science and nanotechnology applications.

X-ray absorption spectroscopy (XAS) is a widely used technique for determining the electronic structure of matter. In contrast to X-ray photoelectron spectroscopy (XPS), XAS makes use of photons only, and therefore suffers less from absorption of the probe beam, i.e., electrons or photons, respectively. This is true for hard X-rays probing, e.g., the Kedges of d-metals in metal hydrides (albeit with limited chemical information). Soft X-rays, which are suited to analyze the electronic structure of hydrogen in solids, have a limited absorption length in gases. Photons with energies of less than 50 eV (“hydrogen K-edge” <;20 eV) are absorbed in less than 1 mm at ambient pressure, which is needed for technical hydrides. Recently, we developed a membrane-based approach to study materials exposed to high hydrogen “pressures” while keeping analysis chamber under high vacuum - thus effectively achieving high pressure XPS analysis. In this paper, we demonstrate that the membrane approach originally designed for XPS can be equally well used for XAS. We show first results on the electronic structure of hydrogen in Pd-Ag alloy as measured by in situ XAS using a laboratory extreme ultraviolet (EUV) source.

Laser plasma soft X-ray sources that operate in the water window and are based on cryogenic targets have been studied. The cryogenic targets used are composed of solid layers of inert gases and are deposition-free targets, which is advantageous for continuous long-lifetime operation using repetitive pulses. The developed laser plasma source has a translating substrate system with a closed He gas cryostat that can continuously supply the cryogenic target, and the source can generate repetitive X-ray pulses continuously. Cryogenic solid Ar and N₂ targets were compared for the soft X-ray source when operating in the water window between 2.3 nm and 4.4 nm. The intensity of the water window Xrays from the Ar target was approximately eight times stronger than that from the N₂ target at a laser intensity of 5×10¹² W/cm² . At this laser intensity, the Ar plasma source also demonstrated a higher conversion efficiency of 14% and an average power of 140 mW in the water window for a laser energy of 1 J at 1 Hz. This power compares favorably with that of X-rays produced using a synchrotron radiation source. The results also indicated that our source satisfied the requirements for use as a source for a contact X-ray microscope. The developed laser plasma source can be used not only for soft X-ray microscopy but also may be used to replace synchrotron facilities in a variety of other applications.

We present an overview of our systematic studies of the surface modifications resulting from the interactions of both single and multiple picosecond soft x-ray laser (SXRL) pulses with materials, such as gold (Au), copper (Cu), aluminum (Al), and lithium fluoride (LiF). We show experimentally the possibility of the precise nanometer size structures (~10–40 nm) formation on their surfaces by ultra-low (~10–30 mJ/cm² ) fluencies of single picosecond SXRL pulse. Comparison experimental results with the atomistic model of ablation, which was developed for the single SXRL shot interaction with dielectrics and metals, is provided. Theoretical description of surface nanostructures is considered and is shown that such structures are formed after laser illumination in a process of mechanical spallation of ultrathin surface layer of molten metal. Spallation is accompanied by a strong foaming of melt, breaking of foam, and freezing of foam remnants. Those remnants form chaotic nanostructures, which are observed in experiments. Our measurements show that electron temperature of matter under irradiation of SXRL was lower than 1 eV. The model calculation also predicts that the ablation induced by the SXRL can create the significant low electron temperature. Our results demonstrate that tensile stress created in LiF and metals by short SXRL pulse can produce spallative ablation of target even for drastically small fluencies, which open new opportunities for material nano processing.

Ultrafast coherent diffraction using soft and hard X-rays is actually revolutionizing imaging science thanks to new sources recently available. This powerful technique extends standard X-ray diffraction towards imaging of non-crystalline objects and leads actually to a strong impact in physics, chemistry and biology. New ultrashort pulses recently available hold the promise of watching matter evolving with unprecedented space and time resolution. Femtosecond coherent and intense radiation in the soft X-ray (λ = 10-40 nm) is currently produced in our laboratory, from highly non linear frequency conversion (high harmonic generation). A high intensity UV-X coherent beam is obtained using a loose focusing geometry, which allows coupling a very high amount of Ti:Sapphire laser system energy in the HHG process. Using a long gas cell and a long focal length lens, the emitting volume can be increased by orders of magnitude compared to standard HHG set-ups. This approach, allows reaching up to 1x1011 photons per shot for the 25th harmonic (λ=32nm). We have already demonstrated nanoscale imaging in a single shot mode reaching 70 nm spatial resolution and 20 femtoseconds snapshot [1]. We then implemented a recently proposed holographic technique using extended references. This technique, easy to implement, allows a direct non iterative image reconstruction. In the single shot regime, we demonstrated a spatial resolution of 110nm [2].This opens fascinating perspectives in imaging dynamical phenomena to be spread over a large scientific community. I will present recent results in the investigation of femtosecond phase spin-reversals of magnetic nano-domains [3]. Finally, I will report on recent development on noise sensitivity of the technique and perspectives in attosecond coherent imaging [4]. [1] A. Ravasio et al., Physical Review Letters 103, 028104 (2009). [2] D. Gauthier et al., Physical Review Letters 105, 093901 (2010). [3] Vodungbo et al., Nature Communications 3, 999 (2012) [4] Williams et al., Optics Letters 40 (13), 3205 (2015)

High-order harmonic generation (HHG) has been recently proven to produce harmonic vortices carrying orbital angular momentum (OAM) in the extreme-ultraviolet (XUV) region from the nonlinear up-conversion of infrared vortex beams. In this work we present two methods to control and extend the OAM content of the harmonic vortices. First, we show that when a driver combination of different vortex modes is used, HHG leads to the production of harmonic vortices with a broad OAM content due to its nonperturbative nature. Second, we show that harmonic vortices with two discrete OAM contributions –so called fractional OAM modes– are generated when HHG is driven by conical refraction beams. Our work offers the possibility of generating tunable OAM beams in the XUV regime, potentially extensible to the soft x rays, overcoming the state of the art limitations for the generation of OAM beams far from the visible domain.

We will present data on a various X-ray production schemes from laser driven plasmas at the PALS Research Center and discuss the plan for the ELI Beamlines project. One of the approaches, how to generate ultrashort pulses of incoherent X-ray radiation, is based on interaction of femtosecond laser pulses with solid or liquid targets. So-called K-alpha source depending on used targets emits in hard X-ray region from micrometric source size. The source exhibits sufficient spatial coherence to observe phase contrast. Detailed characterization of various sources including the x-ray spectrum and the x-ray average yield along with phase contrast images of test objects will be presented. Other method, known as laser wakefield electron acceleration (LWFA), can produce up to GeV electron beams emitting radiation in collimated beam with a femtosecnond pulse duration. This approach was theoretically and experimentally examined at the PALS Center. The parameters of the PALS Ti:S laser interaction were studied by extensive particle-in-cell simulations with radiation post-processors in order to evaluate the capabilities of our system in this field. The extensions of those methods at the ELI Beamlines facility will enable to generate either higher X-ray energies or higher repetition rate. The architecture of such sources and their considered applications will be proposed.

Here we demonstrate performance of an original lab system designed for testing of X-ray parabolic compound refractive lenses (CRL) manufactured from a high-quality single-crystalline synthetic diamond grown by the high-pressure hightemperature technique. The basic parameters of a diamond CRL comprised from 28 plano-concave lenses such as the focal length of 634 mm, transmissivity of 0.36, field of view of ~1 mm and resolution of 6 µm have been determined. Usually such measurements are performed on synchrotron radiation facilities. In this work characterization of CRL was performed by means of instruments and components that are available for laboratories such as the Rigaku 9kW rotating anode X-ray generator, the PANalytical parallel beam X-ray mirror, a 6 m long optical bench, high precision multi-axis goniometers, high resolution X-ray emulsion films, and ultra-fast high-sensitive X-ray area detector PIXel^3D. Developed setup was used to find differences between experimental and design parameters, which is very important for the improvement of CRLs manufacturing technology.

A new type of a high-brilliance X-ray source known as the Thomson X-ray laser-electron generator (TXG) opens new possibilities for materials characterization by X-ray diffraction methods such as high resolution X-ray diffractometry and topography and diffraction analysis at extreme conditions in shear diamond anvil cells. The advantages of the TXG compared to X-ray laboratory sources are a high flux, a quasi-monochromatic, nearly parallel beam and a tunable wavelength. The paper presents examples of applications as well as estimations of typical photon flux and exposure time saving advantages resulted from an implementation of TXG radiation in a home laboratory.

We present lasing in Ni-like molybdenum x-ray laser (18.9 nm) demonstrated with grazing incidence pumping and complete diagnostics of the generated EUV beam. This source of EUV radiation was the first experimental realization of transient x-ray laser at the PALS laboratory. The experiment was performed on a 10 Hz Ti:Sapphire laser system with highly efficient grazing incidence pumping by single beam with profiled laser pulse which included a long prepulse followed by a short main pump pulse. The plasma column was created by focusing of the pumping laser beam on a slab target by a spherical mirror in two different off-axis configurations. Lasing close to saturation with EUV pulses of energy around 100 nJ was demonstrated with less than 500 mJ pumping energy on target. Experimental data from far-field images were analyzed by applying the generalized Van Cittert-Zernike theorem which in general relates field correlation function at the source with intensity in the far-field and can give information about the source size.

There is a quest for new knowledge and methods to study various materials and processes on surfaces and interfaces at the nanoscale. It concerns ablation, phase transitions, physical and chemical transformations, dissolution, selforganization etc. Obviously, to achieve an appropriate resolution it is necessary to use a corresponding wavelength . Higher resolution can be obtained with shorter wavelengths. On the other hand, in surface modification, ablation, study of buried interfaces etc. the penetration length of radiation into the materials, which depends on the wavelength and angle of incidence, plays important role... Considering these factors the experimental studies in nano-physics and nanotechnology are usually carried out using X-ray radiation with a photon energy of 0.1-10 keV. As far as surfaces and films are investigated, it is reasonable to use an X-ray microscope operating in the reflection mode. However, in this spectral range a substantial portion of the radiation is reflected only at small grazing angles (e.g. ≤ 10°). Thus, the idea of grazing incidence reflection-mode X-ray microscope has been developed. In this paper, we consider one of possible schemes of such an X-ray microscope. Our analysis and simulation is based on the extension of the Fresnel propagation theory to tilted object problems.

Laser-produced plasmas are intense sources of XUV radiation that can be suitable for different applications such as extreme ultraviolet lithography, beyond extreme ultraviolet lithography and water window imaging. In particular, much work has focused on the use of tin plasmas for extreme ultraviolet lithography at 13.5 nm. We have investigated the spectral behavior of the laser produced plasmas formed on closely packed polystyrene microspheres and porous alumina targets covered by a thin tin layer in the spectral region from 2.5 to 16 nm. Nd:YAG lasers delivering pulses of 170 ps (Ekspla SL312P )and 7 ns (Continuum Surelite) duration were focused onto the nanostructured targets coated with tin. The intensity dependence of the recorded spectra was studied; the conversion efficiency (CE) of laser energy into the emission in the 13.5 nm spectral region was estimated. We have observed an increase in CE using high intensity 170 ps Nd:YAG laser pulses as compared with a 7 ns pulse.