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Irradiation effects of PMMA induced by femtosecond-pulsed extreme ultraviolet (EUV) were investigated using Soft X-ray free electron laser (SXFEL) for realization of next generation lithography. The sensitivity of PMMA upon exposure to femtosecond-pulsed SXFEL was much higher than that measured for conventional nanosecond-pulsed EUV source. This result speculates the reactions induced by femtosecond-pulsed SXFEL was different from those induced by nanosecond-pulsed EUV.

Silicon polymorphs with exotic electronic and optical properties have recently attracted significant attention due to the wide range of useful bandgap characteristics1,2,3,4. They are typically formed by high pressure techniques, which put limitations on the sample volumes and their crystal structure5,6,7,8,9,10. This constitutes a major obstacle to study these polymorphs and their incorporation into existing technology. Here, we report on a new approach to create unusual crystal structures deep into the bulk of a silicon wafer by MeV-electrons generated by laser irradiation at ultra-relativistic intensity above ~2x10^18 W/cm2. Strong repulsion between the electrons, their branching due to self-generated magnetic field and nonlinear relativistic effects11,12,13 enhance deposition of their energy deep into the target and form high energy density conditions leading to ionisation, followed by fast quenching and restructuring into new crystal arrangements14,15,16,17,18. Analysis by Raman spectroscopy, synchrotron X-ray diffraction, and high-resolution transmission electron microscopy of nanocrystals formed in the irradiated samples provide compelling evidence of the formation of metastable Si phases. The unexplored domain of material transformations exposed to laser-produced MeV-electrons opens new pathways for the conversion into new crystal structures applicable to a wide range of materials at considerably larger quantity, all preserved for further studies and exploitation.

Although laser irradiation with femtosecond pulses is known to generate crystallization and morphological changes, the contribution of optical parameters to material changes is still in discussion. Here, we compare two structures irradiated near Si–L2,3 edges by an extreme ultraviolet femtosecond pulse. Our result implies that, despite the femtosecond irradiation regime, these values of the optical attenuation length between the wavelengths of 10.3-nm and 13.5-nm differ by one order of magnitude. From the structural comparison, the original crystalline state was maintained upon irradiation at 13.5-nm, on the other hand, transition to an amorphous state occurred at 10.3-nm. The difference in optical attenuation length directly influence to the decision of material crystallization or morphological changes, even if the irradiation condition is under the femtosecond regime and same pulse duration. Our result reveals the contribution of optical attenuation length in ultrafast laser-induced structural change.

Extreme conditions inside ice giants such as Uranus and Neptune can result in peculiar chemistry and structural transitions, e.g., the precipitation of diamonds or superionic water, as so far experimentally observed only for pure C─H and H 2 O systems, respectively. Here, we investigate a stoichiometric mixture of C and H 2 O by shock-compressing polyethylene terephthalate (PET) plastics and performing in situ x-ray probing. We observe diamond formation at pressures between 72 ± 7 and 125 ± 13 GPa at temperatures ranging from ~3500 to ~6000 K. Combining x-ray diffraction and small-angle x-ray scattering, we access the kinetics of this exotic reaction. The observed demixing of C and H 2 O suggests that diamond precipitation inside the ice giants is enhanced by oxygen, which can lead to isolated water and thus the formation of superionic structures relevant to the planets’ magnetic fields. Moreover, our measurements indicate a way of producing nanodiamonds by simple laser-driven shock compression of cheap PET plastics.

Focusing of an X-ray free-electron laser enables the production of ultrahigh-intensity X-ray pulses. X-ray nanobeams of a free-electron laser were generated using reflective focusing optics combined with speckle interferometry., Ultimate focusing of an X-ray free-electron laser (XFEL) enables the generation of ultrahigh-intensity X-ray pulses. Although sub-10 nm focusing has already been achieved using synchrotron light sources, the sub-10 nm focusing of XFEL beams remains difficult mainly because the insufficient stability of the light source hinders the evaluation of a focused beam profile. This problem is specifically disadvantageous for the Kirkpatrick–Baez (KB) mirror focusing system, in which a slight misalignment of ∼300 nrad can degrade the focused beam. In this work, an X-ray nanobeam of a free-electron laser was generated using reflective KB focusing optics combined with speckle interferometry. The speckle profiles generated by 2 nm platinum particles were systematically investigated on a single-shot basis by changing the alignment of the multilayer KB mirror system installed at the SPring-8 Angstrom Compact Free-Electron Laser, in combination with computer simulations. It was verified that the KB mirror alignments were optimized with the required accuracy, and a focused vertical beam of 5.8 nm (±1.2 nm) was achieved after optimization. The speckle interferometry reported in this study is expected to be an effective tool for optimizing the alignment of nano-focusing systems and for generating an unprecedented intensity of up to 1022 W cm−2 using XFEL sources.

Proceedings of the National Academy of Sciences of the United States of America 119(12), e2119616119 (2022). doi:10.1073/pnas.2119616119, Coherent nonlinear spectroscopies and imaging in the X-ray domain provide direct insight into the coupled motions of electrons and nuclei with resolution on the electronic length and time scale. The experimental realization of such techniques will strongly benefit from access to intense, coherent pairs of femtosecond X-ray pulses. We have observed phase-stable X-ray pulse pairs containing more than 3*107 photons at 5.9 keV (2.1 ��) with ~1 fs duration and 2-5 fs separation. The highly directional pulse pairs are manifested by interference fringes in the superfluorescent and seeded stimulated manganese K�� emission induced by an X-ray free-electron laser. The fringes constitute the time-frequency X-ray analogue of Young���s double-slit interference allowing for frequency-domain X-ray measurements with attosecond time resolution., Published by National Acad. of Sciences, Washington, DC

Although laser irradiation with femtosecond pulses is known to generate crystallization and morphological changes, the contribution of optical parameters to material changes is still in discussion. Here, we compare two structures irradiated near Si–L2,3 edges by an extreme ultraviolet femtosecond pulse. Our result implies that, despite the femtosecond irradiation regime, these values of the optical attenuation length between the wavelengths of 10.3-nm and 13.5-nm differ by one order of magnitude. From the structural comparison, the original crystalline state was maintained upon irradiation at 13.5-nm, on the other hand, transition to an amorphous state occurred at 10.3-nm. The difference in optical attenuation length directly influence to the decision of material crystallization or morphological changes, even if the irradiation condition is under the femtosecond regime and same pulse duration. Our result reveals the contribution of optical attenuation length in ultrafast laser-induced structural change.

A simple spectrometer using diffraction from diamond microcrystals has been developed to diagnose single-shot spectra of X-ray free-electron laser (XFEL) pulses. The large grain size and uniform lattice constant of the adopted crystals enable characterizing the XFEL spectrum at a resolution of a few eV from the peak shape of the powder diffraction profile. This single-shot spectrometer has been installed at beamline 3 of SACLA and is used for daily machine tuning.

A new method of spatially resolved single-shot absorption spectroscopy for an x-ray free electron laser (XFEL) pulse has been developed by using a dispersive spectrometer and an elliptical mirror to enhance the spatial resolution. As a demonstration, we performed x-ray absorption near-edge structure measurement of Cu with a pump–probe scheme combining an XFEL pulse and a high-power femtosecond laser pulse. In the experiment, changes of an absorption spectrum in a plasma generated with a laser shot were successfully observed. The method will be a powerful tool for experiments requiring a spatial resolution and/or a single-shot measurement, such as high energy density science using a high-power laser pulse.

Control of the polarization of an X-ray free-electron laser (XFEL) has been performed using an X-ray phase retarder (XPR) in combination with an arrival timing diagnostic on BL3 of the SPring-8 Angstrom Compact free-electron LAser (SACLA). To combine with the timing diagnostic, a pink beam was incident on the XPR crystal and then monochromated in the vicinity of samples. A high degree of circular polarization of ∼97% was obtained experimentally at 11.567 keV, which agreed with calculations based on the dynamical theory of X-ray diffraction. This system enables pump–probe experiments to be operated using circular polarization with a time resolution of 40 fs to investigate ultrafast magnetic phenomena.

X-ray free-electron lasers (XFELs)1,2 are widely operated on the basis of self-amplified spontaneous emission (SASE)3,4, where spontaneous radiation from the electron beam is amplified along the magnetic field in undulators. Despite their high intensities, SASE-XFELs have a broad spectrum due to the stochastic starting-up process5. To narrow the bandwidth, self-seeding has been proposed6,7 and recently demonstrated8,9, where the seed pulse produced by monochromatizing the SASE-XFELs from the first section of undulators using a thin crystal in transmission geometry is amplified in the remaining undulators. Here, we present an efficient self-seeding scheme using the Bragg reflection to produce a seed pulse. We applied this scheme to SPring-8 Angstrom Compact free-electron LAser (SACLA)10, and produced nearly Fourier-transform-limited XFEL pulses that correspond to an increase in spectral brightness by a factor of six compared with SASE-XFELs. This achievement will not only enhance the throughput of present XFEL experiments but also should open new opportunities for X-ray science. A nearly Fourier-limited X-ray free-electron laser beam is generated by a self-seeding scheme. The beam in the first half of the undulators is monochromatized via Bragg reflection, and is subsequently amplified in the remaining undulators.

An experimental platform using X-ray free-electron laser (XFEL) pulses with high-intensity optical laser pulses is open for early users' experiments at the SACLA XFEL facility after completion of the commissioning. The combination of the hard XFEL and the high-intensity laser provides capabilities to open new frontiers of laser-based high-energy-density science. During the commissioning phase, characterization of the XFEL and the laser at the platform has been carried out for the combinative utilization as well as the development of instruments and basic diagnostics for user experiments. An overview of the commissioning and the current capabilities of the experimental platform is presented.

Physical review letters 126(11), 117403 (1-6) (2021). doi:10.1103/PhysRevLett.126.117403, Ultrafast changes of charge density distribution in diamond after irradiation with an intense x-ray pulse (photon energy, 7.8 keV; pulse duration, 6 fs; intensity, 3×10$^{19}$ W/cm$^2$) have been visualized with the x-ray pump–x-ray probe technique. The measurement reveals that covalent bonds in diamond are broken and the electron distribution around each atom becomes almost isotropic within ∼5 fs after the intensity maximum of the x-ray pump pulse. The 15 fs time delay observed between the bond breaking and atomic disordering indicates nonisothermality of electron and lattice subsystems on this timescale. From these observations and simulation results, we interpret that the x-ray-induced change of the interatomic potential drives the ultrafast atomic disordering underway to the following nonthermal melting., Published by APS, College Park, Md.

Physical review letters 128(22), 223203 (2022). doi:10.1103/PhysRevLett.128.223203, Transient structural changes of Al$_2$O$_3$ on subatomic length scales following irradiation with an intense x-ray laser pulse (photon energy: 8.70 keV; pulse duration: 6 fs; fluence: 8×10$^2$ J/cm$^2$) have been investigated by using an x-ray pump x-ray probe technique. The measurement reveals that aluminum and oxygen atoms remain in their original positions by ∼20 fs after the intensity maximum of the pump pulse, followed by directional atomic displacements at the fixed unit cell parameters. By comparing the experimental results and theoretical simulations, we interpret that electron excitation and relaxation triggered by the pump pulse modify the potential energy surface and drives the directional atomic displacements. Our results indicate that high-resolution x-ray structural analysis with the accuracy of 0.01 Å is feasible even with intense x-ray pulses by making the pulse duration shorter than the timescale needed to complete electron excitation and relaxation processes, which usually take up to a few tens of femtoseconds., Published by APS, College Park, Md.

To shorten the duration of x-ray pulses, we present a nonlinear optical technique using atoms with core-hole vacancies (core-hole atoms) generated by inner-shell photoionization. The weak Coulomb screening in the core-hole atoms results in decreased absorption at photon energies immediately above the absorption edge. By employing this phenomenon, referred to as saturable absorption, we successfully reduce the duration of x-ray free-electron laser pulses (photon energy: 9.000 keV, duration: 6-7 fs, fluence: 2.0-3.5$\times$10$^5$ J/cm$^2$) by $\sim$35%. This finding that core-hole atoms are applicable to nonlinear x-ray optics is an essential stepping stone for extending nonlinear technologies commonplace at optical wavelengths to the hard x-ray region.

We devised a portable system that generates pulsed high magnetic fields up to 77 T with 3 $\mu$s duration. The system employs the single turn coil method, a destructive way of field generation. The system consists of a capacitor of 10.4 $\mu$F, a 30 kV charger, a mono air-gap switch, a triggering system, and a magnet clamp, which weighs less than 1.0 tons in total and is transportable. The system offers opportunities for single-shot experiments at ultrahigh magnetic fields in combinations with novel quantum beams. The single-shot x-ray diffraction experiment using x-ray free-electron laser at 65 T is presented. We comment on the possible update of the system for the generation of 100 T., Comment: 5 pages, 4 figures

We evaluated laser-induced damage thresholds (LIDTs) on silica glasses by two kinds of ultra-short soft X-ray laser pulses (13.5 nm, 70 fs, and 13.9 nm, 7 ps). The comparison of our experimental results and the reported values observed by nanosecond soft X-ray pulse revealed a pulse width dependence of LIDTs on silica glasses in the soft X-ray region. The relationship between the pulse width and LIDTs provided valuable discussions of the laser-induced damage mechanism.

The extreme pressures achievable with dynamic compression holds great promise for studying planetary interiors. Phase stability of Fe-Si alloys, which are complex to address, is particularly relevant to understanding telluric planetary cores due to the widely varying properties produced by small changes in Si concentration. Here we report the study of phase stability of pure iron and Fe-Si alloys by x-ray diffraction measurements carried out on shocked samples using an x-ray free electron laser (XFEL). Our setup combined with the brilliance of the XFEL allows us to observe the rapid onset of high-pressure solid-solid phase transformation in Fe and Fe-Si8.5wt%; we observe no such evidence in Fe-Si16wt% up to 110 GPa on the nanosecond timescale. Density Functional Theory calculations provide the conceptual framework to rationalize these observations. Taken together our experiments and calculations support recent dynamic compression measurements and shed light on conflicting static compression results. Our work highlights the need to properly consider the differing intrinsic timescales of the static and dynamic experiments when comparing results, and the complementarity of the techniques in assessing phase diagram and transition mechanisms.

We present results from the SPring-8 Angstrom Compact free electron LAser (SACLA) XFEL facility, using a high intensity ($\sim\!10^{20}\,$W/cm$^2$) X-ray pump X-ray probe scheme to observe changes in the ionic structure of silicon induced by X-ray heating of the electrons. By avoiding Laue spots in the scattering signal from a single crystalline sample, we observe a rapid rise in diffuse scattering, which we attribute to a loss of lattice order and a transition to a liquid state within 100 fs of irradiation, a timescale which agrees well with first principles simulations, but is faster than that predicted by purely inertial behavior. This method is capable of observing liquid scattering without masking or filtering of signal from the ambient solid, allowing the liquid structure to be measured throughout and beyond the phase change., 6 pages, 5 figures. Updated title and abstract

A nanofocusing optical system&mdash, referred to as 100 exa&mdash, for an X-ray free-electron laser (XFEL) was developed to generate an extremely high intensity of 100 EW/cm2 (1020 W/cm2) using total reflection mirrors. The system is based on Kirkpatrick-Baez geometry, with 250-mm-long elliptically figured mirrors optimized for the SPring-8 Angstrom Compact Free-Electron Laser (SACLA) XFEL facility. The nano-precision surface employed is coated with rhodium and offers a high reflectivity of 80%, with a photon energy of up to 12 keV, under total reflection conditions. Incident X-rays on the optics are reflected with a large spatial acceptance of over 900 &mu, m. The focused beam is 210 nm &times, 120 nm (full width at half maximum) and was evaluated at a photon energy of 10 keV. The optics developed for 100 exa efficiently achieved an intensity of 1 &times, 1020 W/cm2 with a pulse duration of 7 fs and a pulse energy of 150 &mu, J (25% of the pulse energy generated at the light source). The experimental chamber, which can provide different stage arrangements and sample conditions, including vacuum environments and atmospheric-pressure helium, was set up with the focusing optics to meet the experimental requirements.

The performance of a hard X-ray split-and-delay optical system with a wavefront division scheme has been investigated at SACLA., The performance of a hard X-ray split-and-delay optical (SDO) system with a wavefront division scheme was investigated at the hard X-ray free-electron laser facility SACLA. For the wavefront division, beam splitters made of edge-polished perfect Si(220) crystals were employed. We characterized the beam properties of the SDO system, and investigated its capabilities for beam manipulation and diagnostics. First, it was confirmed that shot-to-shot non-invasive diagnostics of pulse energies for both branches in the SDO system was feasible. Second, nearly ideal and identical focal profiles for both branches were obtained with a spot size of ∼1.5 µm in full width at half-maximum. Third, a spatial overlap of the two focused beams with a sub-µm accuracy was achieved by fine tuning of the SDO system. Finally, a reliable tunability of the delay time between two pulses was confirmed. The time interval was measured with an X-ray streak camera by changing the path length of the variable-delay branch. Errors from the fitted line were evaluated to be as small as ±0.4 ps over a time range of 60 ps.

Meteorites from interplanetary space often include high-pressure polymorphs of their constituent minerals, which provide records of past hypervelocity collisions. These collisions were expected to occur between kilometre-sized asteroids, generating transient high-pressure states lasting for several seconds to facilitate mineral transformations across the relevant phase boundaries. However, their mechanisms in such a short timescale were never experimentally evaluated and remained speculative. Here, we show a nanosecond transformation mechanism yielding ringwoodite, which is the most typical high-pressure mineral in meteorites. An olivine crystal was shock-compressed by a focused high-power laser pulse, and the transformation was time-resolved by femtosecond diffractometry using an X-ray free electron laser. Our results show the formation of ringwoodite through a faster, diffusionless process, suggesting that ringwoodite can form from collisions between much smaller bodies, such as metre to submetre-sized asteroids, at common relative velocities. Even nominally unshocked meteorites could therefore contain signatures of high-pressure states from past collisions., Meteorites from space often include denser polymorphs of their minerals, providing records of past hypervelocity collisions. An olivine mineral crystal was shock-compressed by a high-power laser, and its transformation into denser ringwoodite was time-resolved using an X-ray free electron laser.

Efforts are being focused on increasing the power of extreme ultraviolet (EUV) light sources used in semiconductor manufacturing to increase the throughput. As a result, the investigation of the effect of high power sources on resist materials is a critical issue. A chemically amplified resist (CAR) and a non-CAR were irradiated with 13.5 nm EUV high-flux pulses from a soft X-ray free-electron laser (FEL). In the non-CAR, the positive-tone resist (ZEP520A) exhibited lower sensitivity at high irradiation densities, while the negative-tone resist exhibited a higher sensitivity. In addition, the dose rate did not considerably affect the sensitivity of the CAR.

The temporal coherence of hard X-ray free-electron laser pulses was characterized by capturing single-shot interferograms with a versatile interferometer composed of six separate optical elements. The visibility measurements as a function of time delay revealed a mean coherence time of 5.9 ± 0.7 fs., Temporal coherence is one of the most fundamental characteristics of light, connecting to spectral information through the Fourier transform relationship between time and frequency. Interferometers with a variable path-length difference (PLD) between the two branches have widely been employed to characterize temporal coherence properties for broad spectral regimes. Hard X-ray interferometers reported previously, however, have strict limitations in their operational photon energies, due to the specific optical layouts utilized to satisfy the stringent requirement for extreme stability of the PLD at sub-ångström scales. The work presented here characterizes the temporal coherence of hard X-ray free-electron laser (XFEL) pulses by capturing single-shot interferograms. Since the stability requirement is drastically relieved with this approach, it was possible to build a versatile hard X-ray interferometer composed of six separate optical elements to cover a wide photon energy range from 6.5 to 11.5 keV while providing a large variable delay time of up to 47 ps at 10 keV. A high visibility of up to 0.55 was observed at a photon energy of 10 keV. The visibility measurement as a function of time delay reveals a mean coherence time of 5.9 ± 0.7 fs, which agrees with that expected from the single-shot spectral information. This is the first result of characterizing the temporal coherence of XFEL pulses in the hard X-ray regime and is an important milestone towards ultra-high energy resolutions at micro-electronvolt levels in time-domain X-ray spectroscopy, which will open up new opportunities for revealing dynamic properties in diverse systems on timescales from femto­seconds to nanoseconds, associated with fluctuations from ångström to nanometre spatial scales.

Direct metrology of coherent short-wavelength beamlines is important for obtaining operational beam characteristics at the experimental site. However, since beam-time limitation imposes fast metrology procedures, a multi-parametric metrology from as low as a single shot is desirable. Here a two-dimensional (2D) procedure based on high-resolution Fresnel diffraction analysis is discussed and applied, which allowed an efficient and detailed beamline characterization at the SACLA XFEL. So far, the potential of Fresnel diffraction for beamline metrology has not been fully exploited because its high-frequency fringes could be only partly resolved with ordinary pixel-limited detectors. Using the high-spatial-frequency imaging capability of an irradiated LiF crystal, 2D information of the coherence degree, beam divergence and beam quality factor M 2 were retrieved from simple diffraction patterns. The developed beam metrology was validated with a laboratory reference laser, and then successfully applied at a beamline facility, in agreement with the source specifications.