Observation of electron-induced characteristic x-ray and bremsstrahlung radiation from a waveguide cavity

We demonstrate x-ray generation based on direct emission of spontaneous x-rays into waveguide modes. Photons are generated by electron impact onto a structured anode target, which is formed as an x-ray waveguide or waveguide array. Both emission of characteristic radiation and bremsstrahlung are affected by the changes in mode density induced by the waveguide structure. We investigate how the excited modal pattern depends on the positions of the metal atoms and the distance of the focused electron beam with respect to the waveguide exit side. We compare the results to synchrotron-excited fluorescence. We then discuss how x-ray generation in waveguides can be used to increase the brilliance and directional emission of tabletop x-ray sources, with a corresponding increase in the spatial coherence. On the basis of the Purcell effect, we lastly show that the gain of emission into waveguide modes is governed by the quality factor of the waveguide

A matter of brightness: table-top X-ray generation inside waveguides and X-ray holography with single free-electron laser pulses

X-ray microscopy delivers insights into the structure of optically opaque bulk specimens with high spatial resolution. The source brightness poses a limit on the achievable resolution, however. While table-top X-ray sources are readily available but provide only low brightness, large-facility sources, such as synchrotrons and X-ray free-electron lasers (XFEL), generate radiation with high brightness and high coherence, but are not easily accessible. In this work, we report on and experimentally demonstrate a novel table-top X-ray source concept to generate spatially coherent X-rays with high brightness, that are emitted directly into the modes of a waveguide. Our estimate of the achievable gain increase demonstrates a substantial brightness improvement with respect to other table-top X-ray sources. In another set of experiments, we make use of the high peak brilliance of an XFEL to observe transient states of water under extreme conditions. In a pump-probe scheme, an infrared laser pulse generates a plasma after optical breakdown to seed a cavitation bubble, which we image with a single XFEL pulse. To get access to the pressure distribution within the shockwave of the cavitation bubbles, we calculate the quantitative phase shift based on a tailored phase-retrieval approach. We further complement nanofocus X-ray holography with time-resolved X-ray diffraction to obtain information on the molecular structure of water after dielectric breakdown. This combined approach delivers quantitative information from microscopic to molecular length scales with high temporal resolution.2023-03-2

Semi-transparent central stop in high-resolution X-ray ptychography using Kirkpatrick-Baez focusing

A ptychographic coherent X-ray diffractive imaging (PCDI) experiment has been carried out using 7.9 keV X-rays and Kirkpatrick–Baez focusing mirrors. By introducing a semi-transparent central stop in front of the detector the dynamic range on the detector is increased by about four orders of magnitude. The feasibility of this experimental scheme is demonstrated for PCDI applications with a resolution below 10 nm. The results are compared with reference data and an increase of resolution by a factor of two is obtained, while the deviation of the reconstructed phase map from the reference is below 1%.PeerReviewe

On incoherent diffractive imaging

Incoherent diffractive imaging (IDI) promises structural analysis with atomic resolution based on intensity interferometry of pulsed X‐ray fluorescence emission. However, its experimental realization is still pending and a comprehensive theory of contrast formation has not been established to date. Explicit expressions are derived for the equal‐pulse two‐point intensity correlations, as the principal measured quantity of IDI, with full control of the prefactors, based on a simple model of stochastic fluorescence emission. The model considers the photon detection statistics, the finite temporal coherence of the individual emissions, as well as the geometry of the scattering volume. The implications are interpreted in view of the most relevant quantities, including the fluorescence lifetime, the excitation pulse, as well as the extent of the scattering volume and pixel size. Importantly, the spatiotemporal overlap between any two emissions in the sample can be identified as a crucial factor limiting the contrast and its dependency on the sample size can be derived. The paper gives rigorous estimates for the optimum sample size, the maximum photon yield and the expected signal‐to‐noise ratio under optimal conditions. Based on these estimates, the feasibility of IDI experiments for plausible experimental parameters is discussed. It is shown in particular that the mean number of photons per detector pixel which can be achieved with X‐ray fluorescence is severely limited and as a consequence imposes restrictive constraints on possible applications.Starting from a simple model of stochastic fluorescence emission, a theory is derived of contrast formation and signal‐to‐noise ratio for incoherent diffractive imaging; its feasibility for plausible experimental parameters is discussed. imag

The collapse of a sonoluminescent cavitation bubble imaged with X-ray free-electron laser pulses

Single bubble sonoluminescence (SBSL) is the phenomenon of synchronous light emission due to the violent collapse of a single spherical bubble in a liquid, driven by an ultrasonic field. During the bubble collapse, matter inside the bubble reaches extreme conditions of several gigapascals and temperatures on the order of 10000 K, leading to picosecond flashes of visible light. To this day, details regarding the energy focusing mechanism rely on simulations due to the fast dynamics of the bubble collapse and spatial scales below the optical resolution limit. In this work we present phase-contrast holographic imaging with single x-ray free-electron laser (XFEL) pulses of a SBSL cavitation bubble in water. X-rays probe the electron density structure and by that provide a uniquely new view on the bubble interior and its collapse dynamics. The involved fast time-scales are accessed by sub-100 fs XFEL pulses and a custom synchronization scheme for the bubble oscillator. We find that during the whole oscillation cycle the bubble’s density profile can be well described by a simple step-like structure, with the radius R following the dynamics of the Gilmore model. The quantitatively measured internal density and width of the boundary layer exhibit a large variance. Smallest reconstructed bubble sizes reach down to $R\simeq0.8\,\mu \mathrm{m}$ , and are consistent with spherical symmetry. While we here achieved a spatial resolution of a few 100 nm, the visibility of the bubble and its internal structure is limited by the total x-ray phase shift which can be scaled with experimental parameters

Structural dynamics of water in a supersonic shockwave

We explore the pressure evolution and structural dynamics of transient phase transitions in a microfluidic water jet after laser-induced dielectric breakdown. To this end, we use a combined approach of near-field holography with single femtosecond x-ray free-electron laser pulses and x-ray diffraction. During cavitation and jet breakup, we observe shock wave emission along the jet. The formation of the shockwave is accompanied by pronounced changes in the structure factor of water as an evidence by a shift in the water diffraction peak. This indicates a transition to a high density liquid structure induced by the transient pressure increase

Nanosecond timing and synchronization scheme for holographic pump–probe studies at the MID instrument at European XFEL

Single-pulse holographic imaging at XFEL sources with 1012 photons delivered in pulses shorter than 100 fs reveal new quantitative insights into fast phenomena. Here, a timing and synchronization scheme for stroboscopic imaging and quantitative analysis of fast phenomena on time scales (sub-ns) and length-scales (≲100 nm) inaccessible by visible light is reported. A fully electronic delay-and-trigger system has been implemented at the MID station at the European XFEL, and applied to the study of emerging laser-driven cavitation bubbles in water. Synchronization and timing precision have been characterized to be better than 1 ns

Single-pulse phase-contrast imaging at free-electron lasers in the hard X-ray regime

X-ray free-electron lasers (XFELs) have opened up unprecedented opportunities for time-resolved nano-scale imaging with X-rays. Near-field propagation-based imaging, and in particular near-field holography (NFH) in its high-resolution implementation in cone-beam geometry, can offer full-field views of a specimen's dynamics captured by single XFEL pulses. To exploit this capability, for example in optical-pump/X-ray-probe imaging schemes, the stochastic nature of the self-amplified spontaneous emission pulses, i.e. the dynamics of the beam itself, presents a major challenge. In this work, a concept is presented to address the fluctuating illumination wavefronts by sampling the configuration space of SASE pulses before an actual recording, followed by a principal component analysis. This scheme is implemented at the MID (Materials Imaging and Dynamics) instrument of the European XFEL and time-resolved NFH is performed using aberration-corrected nano-focusing compound refractive lenses. Specifically, the dynamics of a micro-fluidic water-jet, which is commonly used as sample delivery system at XFELs, is imaged. The jet exhibits rich dynamics of droplet formation in the break-up regime. Moreover, pump–probe imaging is demonstrated using an infrared pulsed laser to induce cavitation and explosion of the jet

Pump-probe X-ray holographic imaging of laser-induced cavitation bubbles with femtosecond FEL pulses

Cavitation bubbles can be seeded from a plasma following optical breakdown, by focusing an intense laser in water. The fast dynamics are associated with extreme states of gas and liquid, especially in the nascent state. This offers a unique setting to probe water and water vapor far-from equilibrium. However, current optical techniques cannot quantify these early states due to contrast and resolution limitations. X-ray holography with single X-ray free-electron laser pulses has now enabled a quasi-instantaneous high resolution structural probe with contrast proportional to the electron density of the object. In this work, we demonstrate cone-beam holographic flash imaging of laser-induced cavitation bubbles in water with nanofocused X-ray free-electron laser pulses. We quantify the spatial and temporal pressure distribution of the shockwave surrounding the expanding cavitation bubble at time delays shortly after seeding and compare the results to numerical simulations