We evaluated the capabilities of an intense ultrafast high-harmonic seeded soft X-ray laser at 32.8 nm wavelength regarding single-shot lensless imaging and ptychography. Additionally the wave front at the exit of the laser plasma amplifier is monitored in amplitude and phase using high resolution ptychography and backpropagation techniques.Characterizing the laser plasma amplifier performance depending on the arrival time of the seed pulse with respect to pump pulses provides insight into the light plasma interaction in the soft X-ray range.
Non-linear interactions between light and matter are crucial for widespread applications in physical sciences, life science and engineering. Second harmonic generation (SHG) and sum-frequency generation spectroscopy in the near infrared and optical range have enabled intriguing insights into surface properties and how they influence for instance chemical reactions [1] . Expansion of these methods by developing non-linear X-ray spectroscopies has recently added the capability of studying surfaces [2] , symmetry-breaking [3] and buried interfaces [4] with elemental specificity. However, widespread application is currently limited by access to free-electron laser facilities. Here we report the first generation of second harmonic emission in the extreme ultraviolet (XUV-SHG) at the titanium M-edge. The experiments were carried out with a high-harmonic seeded SXRL [5] bringing nonlinear XUV spectroscopy with atomic specificity to the table-top. The SXRL pulses with an energy of (14 ± 2) nJ, a pulse duration of (1.73 ± 0.13) ps, wavelength of 32.8 nm and a Gaussian-like beam profile is focused down with a gold ellipsoidal mirror down to an elliptical spot with a size of roughly 20 µ m x 40 µ m. The estimated intensity on target is about of (1.0 ± 0.1)•10 10 W/cm 2 . In the focus we exceeded the damage threshold fluence of 2 mJ/cm 2 and observed single-shot damage of 50 nm Ti foils. At these intensities we also generate second harmonic light at 75.6 eV. The fundamental and SHG beams are refocused with a toroidal mirror, spectrally separated by a grating and imaged on a cooled CCD camera.
Time-resolved imaging allows revealing the interaction mechanisms in the microcosm of both inorganic and biological objects. While X-ray microscopy has proven its advantages for resolving objects beyond what can be achieved using optical microscopes, dynamic studies using full-field imaging at the nanometer scale are still in their infancy. In this perspective, we present the current state of the art techniques for full-field imaging in the extreme-ultraviolet- and soft X-ray-regime which are suitable for single exposure applications as they are paramount for studying dynamics in nanoscale systems. We evaluate the performance of currently available table-top sources, with special emphasis on applications, photon flux, and coherence. Examples for applications of single shot imaging in physics, biology, and industrial applications are discussed.
The interaction of intense light with matter gives rise to competing nonlinear responses that can dynamically change material properties. Prominent examples are saturable absorption (SA) and two-photon absorption (TPA), which dynamically increase and decrease the transmission of a sample depending on pulse intensity, respectively. The availability of intense soft X-ray pulses from free-electron lasers (FEL) has led to observations of SA and TPA in separate experiments, leaving open questions about the possible interplay between and relative strength of the two phenomena. Here, we systematically study both phenomena in one experiment by exposing graphite films to soft X-ray FEL pulses of varying intensity, with the FEL energy tuned to match carbon 1s to $\pi^*$ or 1s to $\sigma^*$ transitions. It is observed for lower intensities that the nonlinear contribution to the absorption is dominated by SA attributed to ground-state depletion; for larger intensities ($>10^{14}$ W/cm$^2$), TPA becomes more dominant. The relative strengths of the two phenomena depend in turn on the specific transition driven by the X-ray pulse. Both observations are consistent with our real-time electronic structure calculations. Our results reveal the competing contributions of distinct nonlinear material responses to spectroscopic signals measured in the X-ray regime, demonstrating an approach of general utility for interpreting FEL spectroscopies.
Abstract Understanding the behaviour of matter under conditions of extreme temperature, pressure, density and electromagnetic fields has profound effects on our understanding of cosmologic objects and the formation of the universe. Lacking direct access to such objects, our interpretation of observed data mainly relies on theoretical models. However, such models, which need to encompass nuclear physics, atomic physics and plasma physics over a huge dynamic range in the dimensions of energy and time, can only provide reliable information if we can benchmark them to experiments under well-defined laboratory conditions. Due to the plethora of effects occurring in this kind of highly excited matter, characterizing isolated dynamics or obtaining direct insight remains challenging. High-density plasmas are turbulent and opaque for radiation below the plasma frequency and allow only near-surface insight into ionization processes with visible wavelengths. Here, the output of a high-harmonic seeded laser-plasma amplifier using eight-fold ionized krypton as the gain medium operating at a 32.8 nm wavelength is ptychographically imaged. A complex-valued wavefront is observed in the extreme ultraviolet (XUV) beam with high resolution. Ab initio spatio-temporal Maxwell–Bloch simulations show excellent agreement with the experimental observations, revealing overionization of krypton in the plasma channel due to nonlinear laser-plasma interactions, successfully validating this four-dimensional multiscale model. This constitutes the first experimental observation of the laser ion abundance reshaping a laser-plasma amplifier. The presented approach shows the possibility of directly modelling light-plasma interactions in extreme conditions, such as those present during the early times of the universe, with direct experimental verification.
From fusion dynamics in stars, to terrestrial lightning events, to new prospects of energy production or novel light sources, hot dense plasmas are of importance for an array of physical phenomena. Due to a plethora of correlations in highly excited matter, direct probing of isolated dynamics remains challenging. Here, the 32.8-nm emission of a high-harmonic seeded laser-plasma amplifier (LPA), using eight-fold ionized Krypton as gain medium, is ptychographically imaged in longitudinal direction in the extreme ultraviolet (XUV). In excellent agreement with ab initio spatio-temporal Maxwell-Bloch simulations, an overionization of krypton due to nonlinear laser-plasma interactions is observed. This constitutes the first experimental observation of the laser ion abundance reshaping a laser plasma amplifier. The findings have direct implications for upscaling plasma-based XUV and X-ray sources and allow modeling light-plasma interactions in extreme conditions, similar to those of the early times of the universe, with direct experimental verification.
We report the direct wavefront characterization of an intense ultrafast high-harmonic-seeded soft X-ray laser (λ=32.8 nm) depending on the arrival time of the seed pulses by high-resolution ptychographic imaging and subsequently perform single-shot nanoscale imaging.
Imaging of biological specimen is one of the most important tools to investigate structures and functionalities in organic components. Improving the resolution of images into the nanometer range call for short wavelengths light sources and large aperture optics. Subsequently, the use of extreme ultraviolet light in the range of 2 nm to 5 nm provides high contrast and high resolution imaging, if it is combined with lensless imaging techniques. We describe important parameters for high resolution lensless imaging of biological samples and specify the required light source properties. To overcome radiation based damage of biological specimen, we discuss the concept of ghost imaging and describe a possible setup towards biological imaging in the extreme ultraviolet range.
