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The invention of X-ray interferometers has led to advanced phase-sensing devices that are invaluable in various applications. These include the precise measurement of universal constants, e.g. the Avogadro number, of lattice parameters of perfect crystals, and phase-contrast imaging, which resolves details that standard absorption imaging cannot capture. However, the sensitivity and robustness of conventional X-ray interferometers are constrained by factors, such as fabrication precision, beam quality, and, importantly, noise originating from external sources or the sample itself. In this work, we demonstrate a novel X-ray interferometric method of phase measurement with enhanced immunity to various types of noise, by extending, for the first time, the concept of the SU(1,1) interferometer into the X-ray regime. We use a monolithic silicon perfect crystal device with two thin lamellae to generate correlated photon pairs via spontaneous parametric down-conversion (SPDC). Arrival time coincidence and sum-energy filtration allow a high-precision separation of the correlated photon pairs, which carry the phase information from orders-of-magnitude larger uncorrelated photonic noise. The novel SPDC-based interferometric method presented here is anticipated to exhibit enhanced immunity to vibrations as well as to mechanical and photonic noise, compared to conventional X-ray interferometers. Therefore, this SU(1,1) X-ray interferometer should pave the way to unprecedented precision in phase measurements, with transformative implications for a wide range of applications.

Interaction-free measurement (IFM) is a promising technique for low-dose detection and imaging, offering the unique advantage of probing an object without absorption of the interrogating photons. We propose an experiment to demonstrate IFM in the single x-ray photon regime. The proposed scheme relies on the triple-Laue (LLL) symmetric x-ray interferometer, where each Laue diffraction acts as a lossy beamsplitter. In contrast to many quantum effects which are highly vulnerable to loss, we show that an experimental demonstration of this effect in the x-ray regime is feasible and can achieve high IFM efficiency even in the presence of substantial loss in the system. The latter aspect is claimed to be a general property of IFM based on our theoretical analysis. We scrutinize two suitable detection schemes that offer efficiencies of up to $\eta\sim \frac{1}{2}$. The successful demonstration of IFM with x-rays promises intriguing possibilities for measurements with reduced dose, mainly advantageous for biological samples, where radiation damage is a significant limitation., Comment: 12 pages, 7 figures, comments are welcome

X-ray Fluorescence Ghost Imaging (XRF-GI) was recently demonstrated for x-ray lab sources. It has the potential to reduce acquisition time and deposited dose by choosing their trade-off with spatial resolution, while alleviating the focusing constraints of the probing beam. Here, we demonstrate the realization of synchrotron-based XRF-GI: We present both an adapted experimental setup and its corresponding required computational technique to process the data. This extends the above-mentioned potential advantages of GI to synchrotron XRF imaging. In addition, it enables new strategies to improve resilience against drifts at all scales, and the study of previously inaccessible samples, such as liquids., Comment: 4 pages, 5 figures

Time-resolved X-ray Emission/Absorption Spectroscopy (Tr-XES/XAS) is an informative experimental tool sensitive to electronic dynamics in materials, widely exploited in diverse research fields. Typically, Tr-XES/XAS requires X-ray pulses with both a narrow bandwidth and sub-picosecond pulse duration, a combination that in principle finds its optimum with Fourier transform-limited pulses. In this work, we explore an alternative xperimental approach, capable of simultaneously retrieving information about unoccupied (XAS) and occupied (XES) states from the stochastic fluctuations of broadband extreme ultraviolet pulses of a free-electron laser. We used this method, in combination with singular value decomposition and Tikhonov regularization procedures, to determine the XAS/XES response from a crystalline silicon sample at the L2,3-edge, with an energy resolution of a few tens of meV. Finally, we combined this spectroscopic method with a pump-probe approach to measure structural and electronic dynamics of a silicon membrane. Tr-XAS/XES data obtained after photoexcitation with an optical laser pulse at 390 nm allowed us to observe perturbations of the band structure, which are compatible with the formation of the predicted precursor state of a non-thermal solid-liquid phase transition associated with a bond softening phenomenon.

We demonstrate the measurement of ultrafast dynamics using ghost spectroscopy and a pump-probe approach with an optical pump and a short-wavelength radiation probe. The ghost spectroscopy approach is used to overcome the challenge of the strong intensity and spectrum fluctuations at free-electron lasers and to provide high -spectral resolution, which enables the measurement of small energy shifts in the absorption spectrum. We exploit the high resolution to explore the dynamics of the charge carrier excitations and relaxations and their impact on the photoinduced structural changes in silicon by measuring the variation of the absorption spectrum of a Si(100) membrane near the silicon L2,3 edge and the accompanying edge shifts in response to the optical illumination.

We demonstrate a simple and robust high-resolution ghost spectroscopy approach for x-ray and extreme ultraviolet absorption spectroscopy at free-electron laser sources. Our approach requires an on-line spectrometer before the sample and a downstream bucket detector. We use this method to measure the absorption spectrum of silicon, silicon carbide and silicon nitride membranes in the vicinity of the silicon L2,3-edge. We show that ghost spectroscopy allows the high-resolution reconstruction of the sample spectral response using a coarse energy scan with self-amplified spontaneous emission radiation. For the conditions of our experiment the energy resolution of the ghost-spectroscopy reconstruction is higher than the energy resolution reached by scanning the energy range by narrow spectral bandwidth radiation produced by the seeded free-electron laser. When we set the photon energy resolution of the ghost spectroscopy to be equal to the resolution of the measurement with the seeded radiation, the measurement time with the ghost spectroscopy method is shorter than scanning the photon energy with seeded radiation. The exact conditions for which ghost spectroscopy can provide higher resolution at shorter times than measurement with narrow band scans depend on the details of the measurements and on the properties of the samples and should be addressed in future studies.

We report the observation of a novel nonlinear effect in the hard x-ray range. Upon illuminating Fe and Cu metal foils with intense x-ray pulses tuned near their respective K edges, photons at nearly twice the incoming photon energy are emitted. The signal rises quadratically with the incoming intensity, consistent with two-photon excitation. The spectrum of emitted high-energy photons comprises multiple Raman lines that disperse with the incident photon energy. Upon reaching the double K-shell ionization threshold, the signal strength undergoes a marked rise. Above this threshold, the lines cease dispersing, turning into orescence lines with energies much greater than obtainable by single electron transitions, and additional Raman lines appear. We attribute these processes to electron-correlation mediated multielectron transitions involving double-core hole excitation and various two-electron de-excitation processes to a final state involving one or more L and M core-holes., Comment: 6 pages, 4 figures

We show that the nonlinear interactions between x rays and longer wavelengths in crystals depend strongly on the band structure and related properties. Consequently, these types of interactions can be used as a powerful probe for fundamental properties of crystalline bulk materials. In contrast to previous work that highlighted that these types of nonlinear interactions can provide microscopic information on the valence electrons at the atomic scale resolution, we show that these interactions also contain information that is related to the periodic potential of the crystal. We explain how it is possible to distinguish between the two contributions. Our work indicates on the possibility for the development of novel multi-dimensional pump-probe metrology techniques that will provide spectroscopic information combined with structural information including ultrafast dynamics at the atomic scale.

An X-ray free-electron laser oscillator (XFELO) is a new type of hard X-ray source that would produce fully coherent pulses with meV bandwidth and stable intensity. The XFELO complements existing sources based on self-amplified spontaneous emission (SASE) from high-gain X-ray free-electron lasers (XFEL) that produce ultra-short pulses with broad-band chaotic spectra. This report is based on discussions of scientific opportunities enabled by an XFELO during a workshop held at SLAC on June 29 - July 1, 2016, Comment: 21 pages, 12 figures

X-ray scattering is a weak linear probe of matter. It is primarily sensitive to the position of electrons and their momentum distribution. Elastic X-ray scattering forms the basis of atomic structural determination while inelastic Compton scattering is often used as a spectroscopic probe of both single-particle excitations and collective modes. X-ray free-electron lasers (XFELs) are unique tools for studying matter on its natural time and length scales due to their bright and coherent ultrashort pulses. However, in the focus of an XFEL the assumption of a weak linear probe breaks down, and nonlinear light-matter interactions can become ubiquitous. The field can be sufficiently high that even non-resonant multiphoton interactions at hard X-rays wavelengths become relevant. Here we report the observation of one of the most fundamental nonlinear X-ray-matter interactions, the simultaneous Compton scattering of two identical photons producing a single photon at nearly twice the photon energy. We measure scattered photons with an energy near 18 keV generated from solid beryllium irradiated by 8.8-9.75 keV XFEL pulses. The intensity in the X-ray focus reaches up to 4x20 W/cm2, which corresponds to a peak electric field two orders of magnitude higher than the atomic unit of field-strength and within four orders of magnitude of the quantum electrodynamic critical field. The observed signal scales quadratically in intensity and is emitted into a non-dipolar pattern, consistent with the simultaneous two-photon scattering from free electrons. However, the energy of the generated photons shows an anomalously large redshift only present at high intensities. This indicates that the instantaneous high-intensity scattering effectively interacts with a different electron momentum distribution than linear Compton scattering, with implications for the study of atomic-scale structure and dynamics of matter