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We investigated the role of electronic excitation, relaxation and transport processes in X-ray induced ultrafast demagnetization of magnetic multilayer systems. In what follows, we report on the results obtained with the newly developed modeling tool, XSPIN, which enables nanoscopic description of electronic processes occurring in X-ray irradiated ferromagnetic materials. With this tool, we have studied the specific response of Co/Pt multilayer system irradiated by an ultrafast XUV pulse at the M-edge of Co (photon energy ~ 60 eV). It was previously studied experimentally at the FERMI free-electron-laser facility, using the magnetic small-angle X-ray scattering technique. The XSPIN simulations show that the magnetic scattering signal from cobalt decreases -- on the femtosecond timescales considered -- due to electronic excitation, relaxation and transport processes both in the cobalt and in the platinum layers. The signal decrease scales with the increasing fluence of incoming radiation, following the trend observed in the experimental data. Confirmation of the predominant role of electronic processes for X-ray induced demagnetization in the regime below the structural damage threshold, achieved with our theoretical study, is a step towards quantitative control and manipulation of X-ray induced magnetic processes on femtosecond timescales.

CO2 mineralization not only captures and stores CO2 permanently but also yields value-added products utilized in, for example, the cement industry. CO2 mineralization has been shown to potentially substantially reduce greenhouse gas (GHG) emissions. Realizing CO2 mineralization's potential on a large scale requires a) solid feedstock, b) CO2 sources, c) low-carbon energy, and d) markets for mineralization products. In general, these four requirements of CO2 mineralization are not satisfied at the same location. Thus, the assessment of CO2 mineralization's large-scale potential necessitates the full supply chain considering all requirements for CO2 mineralization simultaneously. At present, neither the potential of CO2 mineralization for GHG emissions reduction on a large scale nor the required supply chain to achieve the potential are fully understood. In our study, we design a climate-optimal supply chain for CO2 capture, utilization, and storage (CCUS) by CO2 mineralization to quantify the large-scale potential of CO2 mineralization in Europe. Our results show that a climate-optimal CCUS by CO2 mineralization could avoid up to 130 Mt CO2e/year of the industrial emissions in Europe even with the current energy supply system. By 2040, CCUS by CO2 mineralization could provide negative emissions of up to 136 Mt CO2e/year. The required energy and CO2 for the CCUS supply chain can be provided either by expanding the current infrastructure by about 5% or, even more climate efficiently, by building new infrastructure. The critical steps toward achieving the large potential of CO2 mineralization in Europe are 1) scaling up the CO2 mineralization technology to the industrial level and 2) exploiting large-scale mineral deposits., Journal of Cleaner Production, 360, ISSN:0959-6526

Ultrashort and intense extreme ultraviolet (XUV) and X-ray pulses readily available at free-electron lasers (FELs) enable studying non-linear light−matter interactions on femtosecond timescales. Here, we report on the non-linear fluence dependence of magnetic scattering of Co/Pt multilayers, using FERMI FEL’s 70-fs-long single and double XUV pulses, the latter with a temporal separation of 200 fs, with a photon energy slightly detuned to the Co M2,3 absorption edge. We observe a quenching in magnetic scattering that sets-in already in the non-destructive fluence regime of a few mJ/cm² typically used for FEL-probe experiments on magnetic materials. Calculations of the transient electronic structure in tandem with a phenomenological modeling of the experimental data by means of ultrafast demagnetization unambiguously show that XUV-radiation-induced demagnetization is the dominant mechanism for the quenching in the investigated fluence regime of

The cement industry emits 7% of the global anthropogenic greenhouse gas (GHG) emissions. Reducing the GHG emissions of the cement industry is challenging since cement production stoichiometrically generates CO

One of the intriguing problems of modern magnetism is unravelling the non-equilibrium spin dynamics following laser excitation on the nanometer length scale. In this work the ultrafast magnetic behavior of thin Co/Pt multilayers is studied by resonant magnetic SAXS in transmission geometry. We have for the first time observed a very bright transient scattering from nanometer scale magnetic fluctuations.

We present a systematic 2D spatial-coherence analysis of the soft-X-ray beamline P04 at PETRA III for various beamline configurations. The influence of two different beam-defining apertures on the spatial coherence properties of the beam is discussed and optimal conditions for coherence-based experiments are found. A significant degradation of the spatial coherence in the vertical direction has been measured and sources of this degradation are identified and discussed. The Fourier-analysis method, which gives fast and simple access to the 2D spatial coherence function of the X-ray beam, is used for the experiment. Here, we exploit the charge scattering of a disordered nanodot sample allowing the use of arbitrary X-ray photon energies with this method.

Condensed Matter 4(3), 77 (2019). doi:10.3390/condmat4030077, In several strongly correlated electron systems, the short range ordering of defects, charge and local lattice distortions are found to show complex inhomogeneous spatial distributions. There is growing evidence that such inhomogeneity plays a fundamental role in unique functionality of quantum complex materials. $\mathrm{La_{1.72}Sr_{0.28}NiO_{4}}$ is a prototypical strongly correlated perovskite showing spin stripes order. In this work we present the spatial distribution of the spin order inhomogeneity by applying micro X-ray diffraction to $\mathrm{La_{1.72}Sr_{0.28}NiO_{4}}$, mapping the spin-density-wave order below the 120 K onset temperature. We find that the spin-density-wave order shows the formation of nanoscale puddles with large spatial fluctuations. The nano-puddle density changes on the microscopic scale forming a multiscale phase separation extending from nanoscale to micron scale with scale-free distribution. Indeed spin-density-wave striped puddles are disconnected by spatial regions with negligible spin-density-wave order. The present work highlights the complex spatial nanoscale phase separation of spin stripes in nickelate perovskites and opens new perspectives of local spin order control by strain., Published by MDPI, Basel

Physical review letters 127(5), 057001 (2021). doi:10.1103/PhysRevLett.127.057001, We study the temporal stability of stripe-type spin order in a layered nickelate with x-ray photon correlation spectroscopy and observe fluctuations on timescales of tens of minutes over a wide temperature range. These fluctuations show an anomalous temperature dependence: they slow down at intermediate temperatures and speed up on both heating and cooling. This behavior appears to be directly connected with spatial correlations: stripes fluctuate slowly when stripe correlation lengths are large and become faster when spatial correlations decrease. A low-temperature decay of nickelate stripe correlations, reminiscent of what occurs in cuprates as a result of a competition between stripes and superconductivity, hence occurs via loss of both spatial and temporal correlations., Published by APS, College Park, Md.

Many fundamental processes in magnetism take place on a nanometer length and sub-picosecond time scale. An important example of such phenomena in magnetism is ultrafast, spin-polarized transport of laser-excited hot electrons, which is now being recognized as playing a crucial role for novel spintronic devices and for optically induced magnetic switching. Recent experimental examples include the demonstration of all-optical helicity dependent control of spin-polarized currents at interfaces [1], the design of novel and efficient terahertz emitters [2], and nanoscale spin reversal in chemically heterogeneous GdFeCo driven by non-local transfer of angular momentum [3]. In particular, for advanced information technologies with bit densities already exceeding 1 terabit per square inch with bit cell dimensions of (15 × 38 nm2) [4], it is of fundamental importance to understand and eventually control the mechanisms responsible for optically induced spin dynamics on the nanoscale.

The results of an X-ray cross-correlation analysis (XCCA) study on hard-sphere colloidal crystals and glasses are presented. The article shows that cross-correlation functions can be used to extract structural information beyond the static structure factor in such systems. In particular, the powder average can be overcome by accessing the crystals' unit-cell structure. In this case, the results suggest that the crystal is of face-centered cubic type. It is demonstrated that XCCA is a valuable tool for X-ray crystallography, in particular for studies on colloidal systems. These are typically characterized by a rather poor crystalline quality due to size polydispersity and limitations in experimental resolution because of the small q values probed. Furthermore, nontrivial correlations are observed that allow a more detailed insight into crystal structures beyond conventional crystallography, especially to extend knowledge in structure formation processes and phase transitions.

Synchrotron radiation news 26(6), 27 - 32 (2013). doi:10.1080/08940886.2013.850384, The free-electron laser (FEL) sources FLASH in Hamburg, LCLS at Stanford, and FERMI in Trieste provide XUV to soft X-ray radiation (FLASH and FERMI) or soft to hard X-ray radiation (LCLS) with unprecedented parameters in terms of ultrashort pulse length, high photon flux, and coherence. These properties make FELs ideal tools for studying ultrafast dynamics in matter on a previously unaccessible level. This paper first reviews results obtained at FEL sources during the last few years in the field of magnetism research. We start with pioneering experiments at FLASH demonstrating the feasibility of magnetic scattering at FELs [1, 2], then present pump–probe scattering experiments [3, 4] as well as the first FEL magnetic imaging experiments [5], and finally discuss a limitation of the scattering methods due to a quenching of the magnetic scattering signal by high-fluence FEL pulses [6]. All of the presented experiments exploit the X-ray magnetic circular dichroism effect [7, 8] to obtain element-specific magnetic scattering contrast, as known from synchrotron experiments [9–12]., Published by Taylor & Francis, Philadelphia, Pa.

We present a method to determine the two-dimensional spatial coherence of synchrotron radiation in the soft X-ray regime by analyzing the Fourier transform of the magnetic speckle pattern from a ferromagnetic film in a multidomain state. To corroborate the results, a Young's double-pinhole experiment has been performed. The transverse coherence lengths in vertical and horizontal direction of both approaches are in a good agreement. The method presented here is simple and gives a direct access to the coherence properties of synchrotron radiation without nanostructured test objects.

It is demonstrated that the magnetic diffraction pattern of the isotropic disordered maze pattern is well described utilizing a gamma distribution of domain sizes in a one-dimensional model. From the analysis, the mean domain size and the shape parameter of the distribution are obtained. The model reveals an average domain size that is significantly different from the value that is determined from the peak position of the structure factor in reciprocal space. As a proof of principle, a wedge-shaped (Co$_{tÅ}$/Pd$_{10Å}$)8 multilayer film, that covers the thickness range of the spin-reorientation transition, has been used. By means of soft x-ray resonant magnetic scattering (XRMS) and imaging techniques the thickness-driven evolution of the magnetic properties of the cobalt layers is explored. It is shown that minute changes of the domain pattern concerning domain size and geometry can be investigated and analyzed due to the high sensitivity and lateral resolution of the XRMS technique. The latter allows for the determination of the magnetic anisotropies of the cobalt layers within a thickness range of a few angstroms.

Scientific Reports 6: Article number: 18970; published online: 06 January 2016; updated: 04 March 2016 The original version of this Article contained a typographical error in the spelling of the author Bharati Tudu, which was incorrectly given as Bahrati Tudu. This has now been corrected in the PDF and HTML versions of the Article.

International audience; Does the excitation of ultrafast magnetization require direct interaction between the photons of the optical pump pulse and the magnetic layer? Here, we demonstrate unambiguously that this is not the case. For this we have studied the magnetization dynamics of a ferromagnetic cobalt/palladium multilayer capped by an IR-opaque aluminum layer. Upon excitation with an intense femtosecond-short IR laser pulse, the film exhibits the classical ultrafast demagnetization phenomenon although only a negligible number of IR photons penetrate the aluminum layer. In comparison with an uncapped cobalt/ palladium reference film, the initial demagnetization of the capped film occurs with a delayed onset and at a slower rate. Both observations are qualitatively in line with energy transport from the aluminum layer into the underlying magnetic film by the excited, hot electrons of the aluminum film. Our data thus confirm recent theoretical predictions. Ultrafast demagnetization is a very intriguing phenomenon. The existence and origin of this rapid loss of a thin film's magnetization on the femtosecond timescale has been controversially debated ever since its discovery in 1996 1. Recently, it has been proposed that the origin of this magnetization loss could be due to spin-dependent motion of the optically excited hot valence electrons causing a spatial redistribution of the magnetization, either to an adjacent metallic layer 2,3 or within the magnetic layer itself 4. Strong experimental evidence for this so-called superdiffusive spin transport has been found lately 5-8. However, the experiment of Eschenlohr and co-workers 8 , similar to our study reported here, has been challenged recently. Khorsand and co-workers 9 showed that the Au cap layer employed in that experiment does not yield the postulated, and for the interpretation of the data crucial, attenuation of the incident IR pump pulse. Implementing a truly IR-opaque capping layer, we evade the limitation affecting the interpretation of the results of Eschenlohr and co-workers 8. Proper characterization of the number of photons reaching the magnetic layer demonstrates that the transmitted intensity is by orders of magnitude too small to excite the ultrafast demagnet-ization process.

International audience; Ultrashort, coherent x-ray pulses of a free-electron laser are used to holographically image the magnetization dynamics within a magnetic domain pattern after creation of a localized excitation via an optical standing wave. We observe a spatially confined reduction of the magnetization within a couple of hundred femtoseconds followed by its slower recovery. Additionally, the experimental results show evidence of a spatial evolution of magnetization, which we attribute to ultrafast transport of nonequilibrium spin-polarized electrons for early times and to a fluence-dependent remagnetization rate for later times.

We present a method to characterize the spatial coherence of soft X-ray radiation from a single diffraction pattern. The technique is based on scattering from non-redundant arrays (NRA) of slits and records the degree of spatial coherence at several relative separations from one to 15 microns, simultaneously. Using NRAs we measured the transverse coherence of the X-ray beam at the XUV X-ray beamline P04 of the PETRA III synchrotron storage ring as a function of different beam parameters. To verify the results obtained with the NRAs additional Young's double pinhole experiments were conducted and show good agreement., Comment: 15 pages, 6 figures, 2 tables, 42 references

FERMI@Elettra, the first vacuum ultraviolet and soft X-ray free-electron laser (FEL) using by default a "seeded" scheme, became operational in 2011 and has been opened to users since December 2012. The parameters of the seeded FERMI FEL pulses and, in particular, the superior control of emitted radiation in terms of spectral purity and stability meet the stringent requirements for single-shot and resonant coherent diffraction imaging (CDI) experiments. The advantages of the intense seeded FERMI pulses with variable polarization have been demonstrated with the first experiments performed using the multipurpose experimental station operated at the diffraction and projection imaging (DiProI) beamline. The results reported here were obtained with fixed non-periodic targets during the commissioning period in 2012 using 20-32 nm wavelength range. They demonstrate that the performance of the FERMI FEL source and the experimental station meets the requirements of CDI, holography, and resonant magnetic scattering in both multi- and single-shot modes. Moreover, we present the first magnetic scattering experiments employing the fully circularly polarized FERMI pulses. The ongoing developments aim at pushing the lateral resolution by using shorter wavelengths provided by double-stage cascaded FERMI FEL-2 and probing ultrafast dynamic processes using different pump-probe schemes, including jitter-free seed laser pump or FEL-pump/FEL-probe with two color FEL pulses generated by the same electron bunch. © 2013 AIP Publishing LLC.

Conditioning therapies before transplantation induce the release of uric acid, which triggers the NLRP3 inflammasome and IL-1β production contributing to graft-versus-host disease., The success of allogeneic hematopoietic cell transplantation is limited by acute graft-versus-host disease (GvHD), a severe complication accompanied by high mortality rates. Yet, the molecular mechanisms initiating this disease remain poorly defined. In this study, we show that, after conditioning therapy, intestinal commensal bacteria and the damage-associated molecular pattern uric acid contribute to Nlrp3 inflammasome–mediated IL-1β production and that gastrointestinal decontamination and uric acid depletion reduced GvHD severity. Early blockade of IL-1β or genetic deficiency of the IL-1 receptor in dendritic cells (DCs) and T cells improved survival. The Nlrp3 inflammasome components Nlrp3 and Asc, which are required for pro–IL-1β cleavage, were critical for the full manifestation of GvHD. In transplanted mice, IL-1β originated from multiple intestinal cell compartments and exerted its effects on DCs and T cells, the latter being preferentially skewed toward Th17. Compatible with these mouse data, increased levels of active caspase-1 and IL-1β were found in circulating leukocytes and intestinal GvHD lesions of patients. Thus, the identification of a crucial role for the Nlrp3 inflammasome sheds new light on the pathogenesis of GvHD and opens a potential new avenue for the targeted therapy of this severe complication.

We present results of single-shot resonant magnetic scattering experiments of $\mathrm{Co}/\mathrm{Pt}$ multilayer systems using 100 fs long ultraintense pulses from an extreme ultraviolet (XUV) free-electron laser. An x-ray-induced breakdown of the resonant magnetic scattering channel during the pulse duration is observed at fluences of $5\text{ }\text{ }\mathrm{J}/{\mathrm{cm}}^{2}$. Simultaneously, the speckle contrast of the high-fluence scattering pattern is significantly reduced. We performed simulations of the nonequilibrium evolution of the $\mathrm{Co}/\mathrm{Pt}$ multilayer system during the XUV pulse duration. We find that the electronic state of the sample is strongly perturbed during the first few femtoseconds of exposure leading to an ultrafast quenching of the resonant magnetic scattering mechanism.

This content may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. This material originally appeared in Review of Scientific Instruments 84, 013906 (2013) and may be found at https://doi.org/10.1063/1.4773543. An endstation for pump–probe small-angle X-ray scattering (SAXS) experiments at the free-electron laser in Hamburg (FLASH) is presented. The endstation houses a solid-state absorber, optical incoupling for pump–probe experiments, time zero measurement, sample chamber, and detection unit. It can be used at all FLASH beamlines in the whole photon energy range offered by FLASH. The capabilities of the setup are demonstrated by showing the results of resonant magnetic SAXS measurements on cobalt-platinum multilayer samples grown on freestanding Si3N4 membranes and pump-laser-induced grid structures in multilayer samples.

Rodlike hematite particles in suspension align perpendicular to an external magnetic field due to a negative anisotropy of their magnetic susceptibility Δχ. The diffusion tensor consists of two principal constants D(∥) and D(⊥) for the diffusion parallel and perpendicular to the long particle axis. X-ray photon correlation spectroscopy is capable of probing the diffusive motion in optically opaque suspensions of rodlike hematite particles parallel to the direction of the scattering vector Q. Choosing Q parallel or perpendicular to the direction of an external magnetic field H the direction dependent intermediate scattering function is measured by means of x-ray photon correlation spectroscopy. From the intermediate scattering function in both directions the principal diffusion constants D(∥) and D(⊥) are determined. The ratio D(∥)/D(⊥) increases with increasing aspect ratio of the particles and can be described via a rescaled theoretical approach for prolate ellipsoids of revolution.

Nature materials 12, 293 - 298 (2013). doi:10.1038/nmat3597, Ultrafast laser techniques have revealed extraordinary spin dynamics in magnetic materials that equilibrium descriptions of magnetism cannot explain. Particularly important for future applications is understanding non-equilibrium spin dynamics following laser excitation on the nanoscale, yet the limited spatial resolution of optical laser techniques has impeded such nanoscale studies. Here we present ultrafast diffraction experiments with an X-ray laser that probes the nanoscale spin dynamics following optical laser excitation in the ferrimagnetic alloy GdFeCo, which exhibits macroscopic all-optical switching. Our study reveals that GdFeCo displays nanoscale chemical and magnetic inhomogeneities that affect the spin dynamics. In particular, we observe Gd spin reversal in Gd-rich nanoregions within the first picosecond driven by the non-local transfer of angular momentum from larger adjacent Fe-rich nanoregions. These results suggest that a magnetic material’s microstructure can be engineered to control transient laser-excited spins, potentially allowing faster (~ 1 ps) spin reversal than in present technologies, Published by Nature Publishing Group, Basingstoke

Physical review letters 108, 267403 (2012). doi:10.1103/PhysRevLett.108.267403, Published by APS, College Park, Md.

The I–V characteristics of amorphous Se thin layers at high applied fields have been found to be I = I 0 exp (− βV 1 2 /kT) . The possible limiting mechanism (Schottky or Poole-Frenkel), corresponding to such a dependence, is analyzed and an explanation based on a particular band model (Simmons) is proposed.

During ultrafast demagnetization of a magnetically ordered solid, angular momentum has to be transferred between the spins, electrons, and phonons in the system on femto- and picosecond timescales. Although the intrinsic spin-transfer mechanisms are intensely debated, additional extrinsic mechanisms arising due to nanoscale heterogeneity have only recently entered the discussion. Here we use femtosecond X-ray pulses from a free-electron laser to study thin film samples with magnetic domain patterns. We observe an infrared-pump-induced change of the spin structure within the domain walls on the sub-picosecond timescale. This domain-topography-dependent contribution connects the intrinsic demagnetization process in each domain with spin-transport processes across the domain walls, demonstrating the importance of spin-dependent electron transport between differently magnetized regions as an ultrafast demagnetization channel. This pathway exists independent from structural inhomogeneities such as chemical interfaces, and gives rise to an ultrafast spatially varying response to optical pump pulses., Ultrafast demagnetization occurs when magnetically ordered solids are exposed to femtosecond light pulses, yet the exact spin-transfer mechanism is still debated. Combining ultrashort X-rays and infrared laser pulses, Pfau et al. show the importance of spin transport between domains in thin magnetic films.

A method for characterization of spatial coherence of X-ray radiation from a single diffraction pattern using non-redundant arrays of slits (NRA) is presented. Using NRAs the spatial coherence of the X-ray beam at the XUV X-ray beamline P04 of the PETRA III storage ring was measured.