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Time-resolved X-ray absorption spectroscopy (tr-XAS) has been shown to be a versatile measurement technique for investigating non-equilibrium dynamics. Novel X-ray free electron laser (XFEL) facilities like the European XFEL offer increased repetition rates for stroboscopic XAS experiments through a burst operation mode, which enables measurements with up to 4.5 MHz. These higher repetition rates lead to higher data acquisition rates but can also introduce long-lived excitations that persist and thus build up during each burst. Here, we report on such long-lived effects in Ni and NiO thin film samples that were measured at the European XFEL. We disentangle the long-lived excitations from the initial pump-induced change and perform a detailed modelling-based analysis of how they modify transient X-ray spectra. As a result, we link the long-lived effects in Ni to a local temperature increase, as well as the effects in NiO to excited charge carrier trapping through polaron formation. In addition, we present possible correction methods, as well as discuss ways in which the effects of these long-lived excitations could be minimized for future time-resolved X-ray absorption spectroscopy measurements.

We present a novel approach to reconstruction of 3D cardiac motion from sparse intraoperative data. While existing methods can accurately reconstruct 3D organ geometries from full 3D volumetric imaging, they cannot be used during surgical interventions where usually limited observed data, such as a few 2D frames or 1D signals, is available in real-time. We propose a versatile framework for reconstructing 3D motion from such partial data. It discretizes the 3D space into a deformable tetrahedral grid with signed distance values, providing implicit unlimited resolution while maintaining explicit control over motion dynamics. Given an initial 3D model reconstructed from pre-operative full volumetric data, our system, equipped with an universal observation encoder, can reconstruct coherent 3D cardiac motion from full 3D volumes, a few 2D MRI slices or even 1D signals. Extensive experiments on cardiac intervention scenarios demonstrate our ability to generate plausible and anatomically consistent 3D motion reconstructions from various sparse real-time observations, highlighting its potential for multimodal cardiac imaging. Our code and model will be made available at https://github.com/Scalsol/MedTet.

We experimentally report on the detection of chaos from a free-running commercial broad-area VCSEL without the need for external perturbation such as optical feedback, injection or current modulation. The evolution of nonlinear dynamics leading to chaotic behavior is studied, and the system's complexity is characterized using chaos titration and correlation dimension. We link the occurence of chaos with the complex interplay between the spatial laser modes competition and polarization dynamics., Comment: 5 pages, 4 figures

Resonant Inelastic X-ray Scattering (RIXS) is an ideal X-ray spectroscopy method to push the combination of energy and time resolutions to the Fourier transform ultimate limit, because it is unaffected by the core-hole lifetime energy broadening. And in pump-probe experiments the interaction time is made very short by the same core-hole lifetime. RIXS is very photon hungry so it takes great advantage from high repetition rate pulsed X-ray sources like the European XFEL. The hRIXS instrument is designed for RIXS experiments in the soft X-ray range with energy resolution approaching the Fourier and the Heisenberg limits. It is based on a spherical grating with variable line spacing (VLS) and a position-sensitive 2D detector. Initially, two gratings are installed to adequately cover the whole photon energy range. With optimized spot size on the sample and small pixel detector the energy resolution can be better than 40 meV at any photon energy below 1000 eV. At the SCS instrument of the European XFEL the spectrometer can be easily positioned thanks to air-pads on a high-quality floor, allowing the scattering angle to be continuously adjusted over the 65-145 deg range. It can be coupled to two different sample interaction chamber, one for liquid jets and one for solids, each equipped at the state-of-the-art and compatible for optical laser pumping in collinear geometry. The measured performances, in terms of energy resolution and count rate on the detector, closely match design expectations. hRIXS is open to public users since the summer of 2022., Comment: 43 pages, 12 figures, Supplemental Material

We experimentally study the synchronization of chaos generated by semiconductor lasers in a cascade injection configuration, i.e., a tunable master laser is used to generate chaos by optical injection in a transmitter laser that injects light into a receiver laser. Chaos synchronization between the transmitter and the receiver lasers is achieved with a correlation coefficient of 90 % for a measurement bandwidth up to 35 GHz. Two parameter regions of good synchronization are found, corresponding to the alignment of the oscillation frequencies of the receiver laser with either the transmitter laser or the master laser., Comment: 5 pages, 6 figures

The photoinduced switching of Fe(II)-based spin-crossover complexes from singlet to quintet takes place at ultrafast time scales. This a priori spin-forbidden transition triggered numerous time-resolved experiments of solvated samples to elucidate the mechanism at play. The involved intermediate states remain uncertain. We apply ultrafast x-ray spectroscopy in molecular films as a method sensitive to spin, electronic, and nuclear degrees of freedom. Combining the progress in molecule synthesis and film growth with the opportunities at x-ray free-electron lasers, we analyze the transient evolution of the Fe L3 fine structure at room temperature. Our measurements and calculations indicate the involvement of an Fe triplet intermediate state. The high-spin state saturates at half of the available molecules, limited by molecule-molecule interaction within the film.

Resonant absorption of a photon by bound electrons in a solid can promote an electron to another orbital state or transfer it to a neighboring atomic site. Such a transition in a magnetically ordered material could affect the magnetic order. While this process is an obvious road map for optical control of magnetization, experimental demonstration of such a process remains challenging. Exciting a significant fraction of magnetic ions requires a very intense incoming light beam, as orbital resonances are often weak compared to above-band-gap excitations. In the latter case, a sizeable reduction of the magnetization occurs as the absorbed energy increases the spin temperature, masking the non-thermal optical effects. Here, using ultrafast x-ray spectroscopy, we were able to resolve changes in the magnetization state induced by resonant absorption of infrared photons in Co-doped yttrium iron garnet, with negligible thermal effects. We found that the optical excitation of the Co ions affects the two distinct magnetic Fe sublattices differently, resulting in a transient non-collinear magnetic state. The present results indicate that the all-optical magnetization switching most likely occurs due to the creation of a transient, non-collinear magnetic state followed by coherent spin rotations of the Fe moments.

The pulse intensity from X-ray free-electron lasers (FELs) can create extreme excitation densities in solids, entering the regime of non-linear X-ray-matter interactions. We show L3-edge absorption spectra of metallic nickel thin films with fluences entering a regime where several X-ray photons are incident per absorption cross-section. Main features of the observed non-linear spectral changes are described with a predictive rate model for electron population dynamics during the pulse, utilizing a fixed density of states and tabulated ground-state properties., Comment: The main text contains 5 pages and 4 figures, the total length including supplement is 14 pages, 7 figures and one table. See also the simultaneously submitted paper about the rate model

The objective of this paper is to describe the implication of an interdisciplinary team involved during a user-centered design methodology to design the platform (WebSoKeyTo) that meets the needs of therapists to design augmentative and alternative communication (AAC) aids for disabled users. We describe the processes of the design process and the role of the various actors (therapists and human computer researchers) in the various phases of the process. Finally, we analyze a satisfaction scale of the therapists on their participation in the codesign process. This study demonstrates the interest in extending the design actors to other therapists and caregivers (professional and family) in the daily life of people with disabilities.

We describe a co-design approach to design the online WebSoKeyTo used to design AAC. This co-design was carried out between a team of therapists and a team of human-computer interaction researchers. Our approach begins with the use and evaluation of an existing SoKeyTo AAC design application. This step was essential in the awareness and definition of the needs by the therapists and in the understanding of the poor usability scores of SoKeyTo by the researchers. We then describe the various phases (focus group, brainstorming, prototyping) with the co-design choices retained. An evaluation of WebSoKeyTo is in progress.

Femtosecond transient soft X-ray Absorption Spectroscopy (XAS) is a very promising technique that can be employed at X-ray Free Electron Lasers (FELs) to investigate out-of-equilibrium dynamics for material and energy research. Here we present a dedicated setup for soft X-rays available at the Spectroscopy & Coherent Scattering (SCS) instrument at the European X-ray Free Electron Laser (EuXFEL). It consists of a beam-splitting off-axis zone plate (BOZ) used in transmission to create three copies of the incoming beam, which are used to measure the transmitted intensity through the excited and unexcited sample, as well as to monitor the incoming intensity. Since these three intensity signals are detected shot-by-shot and simultaneously, this setup allows normalized shot-by-shot analysis of the transmission. For photon detection, the DSSC imaging detector, which is capable of recording up to 800 images at 4.5 MHz frame rate during the FEL burst, is employed and allows approaching the photon shot-noise limit. We review the setup and its capabilities, as well as the online and offline analysis tools provided to users., Comment: 11 figures

The complex electronic structure of metallic ferromagnets is determined by a balance between exchange interaction, electron hopping leading to band formation, and local Coulomb repulsion. The interplay between the respective terms of the Hamiltonian is of fundamental interest, since it produces most, if not all, of the exotic phenomena observed in the solid state. By combining high energy and temporal resolution in femtosecond time-resolved X-ray absorption spectroscopy with ab initio time-dependent density functional theory we analyze the electronic structure in fcc Ni on the time scale of these interactions in a pump-probe experiment. We distinguish transient broadening and energy shifts in the absorption spectra, which we demonstrate to be caused by electron repopulation and correlation-induced modifications of the electronic structure, respectively. Importantly, the theoretical description of this experimental result hence requires to take the local Coulomb interaction into account, revealing a temporal interplay between band formation, exchange interaction, and Coulomb repulsion.

The SASE3 soft X-ray beamline at the European XFEL has been designed and built to provide experiments with pink or monochromatic beam in the photon energy range 250 eV - 3000 eV. Here, we focus on the monochromatic operation of the SASE3 beamline and report on design and performance of the SASE3 grating monochromator. The unique capability of an FEL source to produce short femtosecond pulses of high degree of coherence challenges the monochromator design by a demand to control both photon energy and temporal resolution. The aim to transport close to transform-limited pulses poses very high demands on the optics quality, in particular on the grating. The current realization of the SASE3 monochromator is discussed in comparison with optimal design performance. Presently, the monochromator operates with two gratings: the low-resolution grating is optimized for time-resolved experiments and allows for moderate resolving power of about 2000 - 5000 along with pulse stretching of few to few tens of femtoseconds RMS, and the high-resolution grating reaches resolving power of 10000 at a cost of larger pulse stretching.

The advent of X-ray free-electron lasers (XFELs) has revolutionized fundamental science, from atomic to condensed matter physics, from chemistry to biology, giving researchers access to X-rays with unprecedented brightness, coherence, and pulse duration. All XFEL facilities built until recently provided X-ray pulses at a relatively low repetition rate, with limited data statistics. Here, we present the results from the first megahertz repetition rate X-ray scattering experiments at the Spectroscopy and Coherent Scattering (SCS) instrument of the European XFEL. We illustrate the experimental capabilities that the SCS instrument offers, resulting from the operation at MHz repetition rates and the availability of the novel DSSC 2D imaging detector. Time-resolved magnetic X-ray scattering and holographic imaging experiments in solid state samples were chosen as representative, providing an ideal test-bed for operation at megahertz rates. Our results are relevant and applicable to any other non-destructive XFEL experiments in the soft X-ray range., Comment: 13 pages, 5 figures. Supplementary Information as ancillary file

Symmetry is a powerful concept in physics, but its applicability to far-from-equilibrium states is still being understood. Recent attention has focused on how far-from-equilibrium states lead to spontaneous symmetry breaking. Conversely, ultrafast optical pumping can be used to drastically change the energy landscape and quench the magnetic order parameter in magnetic systems. Here, we find a distinct symmetry-dependent ultrafast behaviour by use of ultrafast x-ray scattering from magnetic patterns with varying degrees of isotropic and anisotropic symmetry. After pumping with an optical laser, the scattered intensity reveals a radial shift exclusive to the isotropic component and exhibits a faster recovery time from quenching for the anisotropic component. These features arise even when both symmetry components are concurrently measured, suggesting a correspondence between the excitation and the magnetic order symmetry. Our results underline the importance of symmetry as a critical variable to manipulate the magnetic order in the ultrafast regime.

Magnetic nanoparticles such as FePt in the L10-phase are the bedrock of our current data storage technology. As the grains become smaller to keep up with technological demands, the superparamagnetic limit calls for materials with higher magneto-crystalline anisotropy. This in turn reduces the magnetic exchange length to just a few nanometers enabling magnetic structures to be induced within the nanoparticles. Here we describe the existence of spin-wave solitons, dynamic localized bound states of spin-wave excitations, in FePt nanoparticles. We show with time-resolved X-ray diffraction and micromagnetic modeling that spin-wave solitons of sub-10 nm sizes form out of the demagnetized state following femtosecond laser excitation. The measured soliton spin-precession frequency of 0.1 THz positions this system as a platform to develop miniature devices capable of filling the THz gap., Comment: 32 pages, please check the "attachemnts" tab in the pdf file in order to see the movie

A change of orbital state alters the coupling between ions and their surroundings drastically. Orbital excitations are hence key to understand and control interaction of ions. Rare-earth (RE) elements with strong magneto-crystalline anisotropy (MCA) are important ingredients for magnetic devices. Thus, control of their localized 4f magnetic moments and anisotropy is one major challenge in ultrafast spin physics. With time-resolved X-ray absorption and resonant inelastic scattering experiments, we show for Tb metal that 4f-electronic excitations out of the ground state multiplet occur after optical pumping. These excitations are driven by inelastic 5d-4f-electron scattering, alter the 4f-orbital state and consequently the MCA with important implications for magnetization dynamics in 4f-metals, and more general for the excitation of localized electronic states in correlated materials., Comment: Manuscript (23 pages, 5 figures) and Supplementary Information (32 pages, 10 figures)

Credit Default Swap (CDS) levels provide a market appreciation of companies' default risk. These derivatives are not always available, creating a need for CDS approximations. This paper offers a simple, global and transparent CDS structural approximation, which contrasts with more complex and proprietary approximations currently in use. This Equity-to-Credit formula (E2C), inspired by CreditGrades, obtains better CDS approximations, according to empirical analyses based on a large sample spanning 2016-2018. A random forest regression run with this E2C formula and selected additional financial data results in an 87.3% out-of-sample accuracy in CDS approximations. The transparency property of this algorithm confirms the predominance of the E2C estimate, and the impact of companies' debt rating and size, in predicting their CDS.

We present a comprehensive experimental and theoretical study on superfluorescence in the extreme ultraviolet wavelength regime. Focusing a high-intensity free-electron laser pulse in a cell filled with Xe or Kr gas, the medium is quasi instantaneously population-inverted by inner-shell ionization on the giant resonance followed by Auger decay. On the timescale of 100 ps a macroscopic polarization builds up in the medium, resulting in superfluorescent emission of several Xe and Kr lines in the forward direction. As the number of emitters in the system is increased by either raising the pressure or the pump-pulse energy, the emission shows an exponential growth of over 4 orders of magnitude and reaches saturation. With increasing yield, we observe line broadening, a manifestation of superfluorescence in the spectral domain. Our novel theoretical approach, based on a full quantum treatment of the atomic system and the irradiated field, shows quantitative agreement with the experiment and supports our interpretation.

The estimation of the extremal dependence structure is spoiled by the impact of the bias, which increases with the number of observations used for the estimation. Already known in the univariate setting, the bias correction procedure is studied in this paper under the multivariate framework. New families of estimators of the stable tail dependence function are obtained. They are asymptotically unbiased versions of the empirical estimator introduced by Huang [Statistics of bivariate extremes (1992) Erasmus Univ.]. Since the new estimators have a regular behavior with respect to the number of observations, it is possible to deduce aggregated versions so that the choice of the threshold is substantially simplified. An extensive simulation study is provided as well as an application on real data., Comment: Published at http://dx.doi.org/10.1214/14-AOS1305 in the Annals of Statistics (http://www.imstat.org/aos/) by the Institute of Mathematical Statistics (http://www.imstat.org)

We present theoretical and experimental results of L\'evy flights of light originating from a random walk of photons in a hot atomic vapor. In contrast to systems with quenched disorder, this system does not present any correlations between the position and the step length of the random walk. In an analytical model based on microscopic first principles including Doppler broadening we find anomalous L\'evy-type superdiffusion corresponding to a single-step size distribution P(x) proportional to x^(-1-alpha), with alpha=1. We show that this step size distribution leads to a violation of Ohm's law [T_(diff) proportional to L^(-alpha/2) different from 1/L], as expected for a L\'evy walk of independent steps. Furthermore the spatial profile of the transmitted light develops power law tails [I(r) proportional to r^(-3-alpha)]. In an experiment using a slab geometry with hot rubidium vapor, we measured the total diffuse transmission T_(diff) and the spatial profile of the transmitted light T_{diff}(r). We obtained the microscopic L\'evy parameter alpha under macroscopic multiple scattering conditions paving the way to investigation of L\'evy flights in different atomic physics and astrophysics systems.

We investigate multiple scattering of near-resonant light in a Doppler-broadened atomic vapor. We experimentally characterize the length distribution of the steps between successive scattering events. The obtained power law is characteristic of a superdiffusive behavior, where rare but very long steps (L\'evy flights) dominate the transport properties., Comment: High resolutions figures in the published version

Conventional lasers make use of optical cavities to provide feedback to gain media. Conversely, mirrorless lasers can be built by using disordered structures to induce multiple scattering, which increases the effective path length in the gain medium and thus provides the necessary feedback. These so-called random lasers potentially offer a new and simple mean to address applications such as lighting. To date, they are all based on condensed-matter media. Interestingly, light or microwave amplification by stimulated emission occurs also naturally in stellar gases and planetary atmospheres. The possibility of additional scattering-induced feedback (that is, random lasing) has been discussed and could explain unusual properties of some space masers. Here, we report the experimental observation of random lasing in a controlled, cold atomic vapour, taking advantage of Raman gain. By tuning the gain frequency in the vicinity of a scattering resonance, we observe an enhancement of the light emission of the cloud due to random lasing. The unique possibility to both control the experimental parameters and to model the microscopic response of our system provides an ideal test bench for better understanding natural lasing sources, in particular the role of resonant scattering feedback in astrophysical lasers.

In this paper, we use steady-state measurements to obtain evidence of radiation trapping in an optically thick a cloud of cold rubidium atoms. We investigate the fluorescence properties of our sample, pumped on opened transitions. The intensity of fluorescence exhibits a non trivial dependence on the optical thickness of the media. A simplified model, based on rate equations self-consistently coupled to a diffusive model of light transport, is used to explain the experimental observations in terms of incoherent radiation trapping on one spectral line. Measurements of atomic populations and fluorescence spectrum qualitatively agree with this interpretation., Comment: 8 pages, 5 figures

The multiple scattering of photons in a hot, resonant, atomic vapor is investigated and shown to exhibit a L\'evy Flight-like behavior. Monte Carlo simulations give insights into the frequency redistribution process that originates the long steps characteristic of this class of random walk phenomena.

Atoms can scatter light and they can also amplify it by stimulated emission. From this simple starting point, we examine the possibility of realizing a random laser in a cloud of laser-cooled atoms. The answer is not obvious as both processes (elastic scattering and stimulated emission) seem to exclude one another: pumping atoms to make them behave as amplifier reduces drastically their scattering cross-section. However, we show that even the simplest atom model allows the efficient combination of gain and scattering. Moreover, supplementary degrees of freedom that atoms offer allow the use of several gain mechanisms, depending on the pumping scheme. We thus first study these different gain mechanisms and show experimentally that they can induce (standard) lasing. We then present how the constraint of combining scattering and gain can be quantified, which leads to an evaluation of the random laser threshold. The results are promising and we draw some prospects for a practical realization of a random laser with cold atoms., Comment: Accepcted for publication by J. Opt. A for the special issue on nanolasers and random lasers (to be published early 2010)

Properties of random and fluctuating systems are often studied through the use of Gaussian distributions. However, in a number of situations, rare events have drastic consequences, which can not be explained by Gaussian statistics. Considerable efforts have thus been devoted to the study of non Gaussian fluctuations such as L\'evy statistics, generalizing the standard description of random walks. Unfortunately only macroscopic signatures, obtained by averaging over many random steps, are usually observed in physical systems. We present experimental results investigating the elementary process of anomalous diffusion of photons in hot atomic vapours. We measure the step size distribution of the random walk and show that it follows a power law characteristic of L\'evy flights., Comment: This final version is identical to the one published in Nature Physics

We address the problem of achieving a random laser with a cloud of cold atoms, in which gain and scattering are provided by the same atoms. In this system, the elastic scattering cross-section is related to the complex atomic polarizability. As a consequence, the random laser threshold is expressed as a function of this polarizability, which can be fully determined by spectroscopic measurements. We apply this idea to experimentally evaluate the threshold of a random laser based on Raman gain between non-degenerate Zeeman states and find a critical optical thickness on the order of 200, which is within reach of state-of-the-art cold-atom experiments.