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-edge resonant inelastic x-ray scattering
摘要： We report an Fe L-edge resonant inelastic x-ray scattering (RIXS) study of the unusual superconductor β-FeSe. The high-energy resolution of this RIXS experiment (≈55 meV FWHM) made it possible to resolve low-energy excitations of the Fe 3d manifold. These include a broad peak which shows dispersive trends between 100 and 200 meV along the (π, 0) and (π, π) directions of the one-Fe square reciprocal lattice, and which can be attributed to paramagnon excitations. The multiband valence state of FeSe is among the most metallic in which such excitations have been discerned by soft x-ray RIXS.
关键词： RIXS,β-FeSe,Fe L-edge,dispersion,paramagnon,superconductor,resonant inelastic x-ray scattering
更新于2025-09-23 15:23:52
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Quantitative Measure of the Size Dispersity in Ultrasmall Fluorescent Organic-Inorganic Hybrid Core-Shell Silica Nanoparticles by Small-angle X-ray Scattering
摘要： Small-angle X-ray scattering (SAXS) was performed on dispersions of ultrasmall (d < 10 nm) fluorescent organic-inorganic hybrid core-shell silica nanoparticles synthesized in aqueous solutions (C′ dots) by using an oscillating flow cell to overcome beam induced particle degradation. Form factor analysis and fitting was used to determine the size and size dispersity of the internal silica core containing covalently encapsulated fluorophores. The structure of the organic poly(ethylene glycol) (PEG) shell was modelled as a monodisperse corona containing concentrated and semi-dilute regimes of decaying density and as a simple polydisperse shell to determine the bounds of dispersity in the overall hybrid particle. C′ dots containing single growth step silica cores have dispersities of 0.19-0.21; growth of additional silica shells onto the core produces a thin, dense silica layer, and increases the dispersity to 0.22-0.23. Comparison to FCS and DLS measures of size shows good agreement with SAXS measured and modelled sizes and size dispersities. Finally, comparison of a set of same sized and purified particles demonstrates that SAXS is sensitive to the skewness of the gel permeation chromatography elugrams of the original as-made materials. These and other insights provided by quantitative SAXS assessments may become useful for generation of robust nanoparticle design criteria necessary for their successful and safe use, for example in nanomedicine and oncology applications.
关键词： nanomedicine,size dispersity,core-shell nanoparticles,silica nanoparticles,Small-angle X-ray scattering,PEGylation
更新于2025-09-23 15:23:52
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Resolving the nature of electronic excitations in resonant inelastic x-ray scattering
摘要： The study of elementary bosonic excitations is essential toward a complete description of quantum electronic solids. In this context, resonant inelastic x-ray scattering (RIXS) has recently risen to becoming a versatile probe of electronic excitations in strongly correlated electron systems. The nature of the radiation-matter interaction endows RIXS with the ability to resolve the charge, spin, and orbital nature of individual excitations. However, this capability has been only marginally explored to date. Here, we demonstrate a systematic method for the extraction of the character of excitations as imprinted in the azimuthal dependence of the RIXS signal. Using this approach, we resolve the charge, spin, and orbital nature of elastic scattering, (para-)magnon/bimagnon modes, and higher-energy dd excitations in magnetically ordered and superconducting copper oxide perovskites (Nd2CuO4 and YBa2Cu3O6.75). Our method derives from a direct application of scattering theory, enabling us to deconstruct the complex scattering tensor as a function of energy loss. In particular, we use the characteristic tensorial nature of each excitation to precisely and reliably disentangle the charge and spin contributions to the low-energy RIXS spectrum. This procedure enables to separately track the evolution of spin and charge spectral distributions in cuprates with doping. Our results demonstrate a new capability that can be integrated into the RIXS toolset and that promises to be widely applicable to materials with intertwined spin, orbital, and charge excitations.
关键词： spin,resonant inelastic x-ray scattering,cuprates,azimuthal dependence,RIXS,electronic excitations,orbital,charge
更新于2025-09-23 15:22:29
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Resonant inelastic x-ray incarnation of Young’s double-slit experiment
摘要： Young’s archetypal double-slit experiment forms the basis for modern diffraction techniques: The elastic scattering of waves yields an interference pattern that captures the real-space structure. Here, we report on an inelastic incarnation of Young’s experiment and demonstrate that resonant inelastic x-ray scattering (RIXS) measures interference patterns, which reveal the symmetry and character of electronic excited states in the same way as elastic scattering does for the ground state. A prototypical example is provided by the quasi-molecular electronic structure of insulating Ba3CeIr2O9 with structural Ir dimers and strong spin-orbit coupling. The double “slits” in this resonant experiment are the highly localized core levels of the two Ir atoms within a dimer. The clear double-slit-type sinusoidal interference patterns that we observe allow us to characterize the electronic excitations, demonstrating the power of RIXS interferometry to unravel the electronic structure of solids containing, e.g., dimers, trimers, ladders, or other superstructures.
关键词： Resonant inelastic x-ray scattering,quasi-molecular orbitals,electronic excitations,Young's double-slit experiment,spin-orbit coupling,interference patterns
更新于2025-09-23 15:22:29
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Ultrathin Y <sub/>2</sub> O <sub/>3</sub> :Eu <sup>3+</sup> nanodiscs: spectroscopic investigations and evidence for reduced concentration quenching
摘要： Here, we report the synthesis and spectral properties of ultrathin nanodiscs (NDs) of Y2O3:Eu3+. It was found that the NDs of Y2O3:Eu3+ with a thickness of about 1 nm can be fabricated in a reproducible, facile and self-assembling process, which does not depend on the Eu3+ concentration. The thickness and morphology of these NDs were determined with small angle x-ray scattering and transmission electron microscopy. We found that the crystal field in these nanoparticles deviates from both the cubic and monoclinic characteristics, albeit the shape of the 5D0 → 7FJ (J = 0, 1, 2) transitions shows some similarity with the transitions in the monoclinic material. The Raman spectra of the non-annealed NDs manifest various vibration modes of the oleic acid molecules, which are used to stabilise the NDs. The annealed NDs show two very weak Raman lines, which may be assigned to vibrational modes of Y2O3 NDs. The concentration quenching of the Eu3+ luminescence of the NDs before annealing is largely suppressed and might be explained in terms of a reduction of the phonon density of states.
关键词： nanodiscs,small angle x-ray scattering,europium-doped yttrium oxide,Raman spectroscopy,concentration quenching,transmission electron microscopy,luminescence
更新于2025-09-23 15:21:21
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<i>In situ</i> structural kinetics of picosecond laser-induced heating and fragmentation of colloidal gold spheres
摘要： Fragmentation of colloidal 54 nm gold nanoparticles by picosecond laser pulses is recorded by time-resolved X-ray scattering, giving access to structural dynamics down to a 80 ps resolution. Lattice temperature and energy dissipation have been quantified to verify that the maximum applied fluence of 1800 J m?2 heats up the particles close to boiling. Already within 30 ns, particles with significantly lower particle sizes of 2 to 3 nm are detected, which hints towards an ultrafast process either by a thermal phase explosion or Coulomb instability. An arrested growth is observed on a microsecond time scale resulting in a final particle size of 3–4 nm with high yield. In this context, the fragmentation in a NaCl/NaOH solution seems to limit growth by electrostatic stabilization of fragments, whereas it does not modify the initial product sizes. The laser-induced fragmentation process is identified as a single-step, instantaneous reaction.
关键词： Coulomb instability,fragmentation,thermal phase explosion,time-resolved X-ray scattering,picosecond laser pulses,gold nanoparticles
更新于2025-09-23 15:21:01
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Binary Superlattices of Infrared Plasmonic and Excitonic Nanocrystals
摘要： Self-assembled superlattices of nanocrystals offer exceptional control over the coupling between nanocrystals, similar to how solid-state crystals tailor the bonding between atoms. By assembling nanocrystals of different properties (e.g., plasmonic, excitonic, dielectric, or magnetic), we can form a wealth of binary superlattice metamaterials with new functionalities. Here, we introduce infrared plasmonic Cu2?xS nanocrystals to the limited library of materials that have been successfully incorporated into binary superlattices. We are the first to create a variety of binary superlattices with large excitonic (PbS) nanocrystals and small plasmonic (Cu2?xS) nanocrystals, both resonant in the infrared. Then, by controlling the surface chemistry of large Cu2?xS nanocrystals, we produced structurally analogous superlattices of large Cu2?xS and small PbS nanocrystals. Transmission electron microscopy (TEM) and grazing-incidence small-angle X-ray scattering (GISAXS) were used to characterize both types of superlattices. Furthermore, our unique surface modification of the large Cu2?xS nanocrystals also prevented them from chemically quenching the photoluminescence of the PbS nanocrystals, which occurred when the PbS nanocrystals were mixed with unmodified Cu2?xS nanocrystals. These synthetic achievements create a set of binary superlattices that can be used to understand how infrared plasmonic and excitonic nanocrystals couple in a variety of symmetries and stoichiometries.
关键词： infrared quantum dots,nanocrystals,self-assembly,supracrystal,metamaterial,binary superlattice,grazing-incidence small-angle X-ray scattering (GISAXS)
更新于2025-09-23 15:21:01
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Kinetics of Ion-Exchange Reactions in Hybrid Organic-Inorganic Perovskite Thin Films Studied by In Situ Real-Time X-ray Scattering
摘要： The exchange of ions in hybrid organic-inorganic perovskites with the general formula APbX3 (A = MA, FA; X = I, Cl, Br) is studied in five different systems using in situ real-time grazing incident X-ray diffraction (GIXD). In systems where the organic cation is exchanged, we find a continuous shift of the lattice parameter. The relative shift compared to the pure materials is used to quantify the exchange. Whether or not a conversion is possible, as well as the amount of exchanged cations, depends on the halide used. In the case of the interconversion of MAPbI3 and MAPbCl3, we observe a decay of the diffraction peaks of the original perovskite and the emergence of new peaks corresponding to the structure with the alternative halide. Moreover, we determined the relevant time scales of the growth and decay of the perovskite structures.
关键词： ion-exchange reactions,kinetics,in situ real-time X-ray scattering,thin films,hybrid organic-inorganic perovskites
更新于2025-09-23 15:21:01
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The GALAXIES inelastic hard X-ray scattering end-station at Synchrotron SOLEIL
摘要： GALAXIES is an in-vacuum undulator hard X-ray micro-focused beamline dedicated to the study of the electronic structure of materials with high energy resolution using both photoelectron spectroscopy and inelastic X-ray scattering and under both non-resonant (NR-IXS) and resonant (RIXS) conditions. Due to the penetrating power of hard X-rays and the ‘photon-in/photon-out’ technique, the sample environment is not a limitation. Materials under extreme conditions, for example in diamond anvil cells or catalysis chambers, thus constitute a major research direction. Here, the design and performance of the inelastic X-ray scattering end-station that operates in the energy range from (cid:2) 4 keV up to 12 keV is reported, and its capabilities are highlighted using a selection of data taken from recently performed experiments. The ability to scan ‘on the fly’ the incident and scattered/emitted X-ray energies, and the sample position enables fast data collection and high experimental throughput. A diamond X-ray transmission phase retarder, which can be used to generate circularly polarized light, will also be discussed in the light of the recent RIXS–MCD approach.
关键词： GALAXIES beamline,beamlines,inelastic hard X-ray scattering,Synchrotron SOLEIL
更新于2025-09-23 15:19:57
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Stimulated resonant inelastic x-ray scattering with chirped, broadband pulses
摘要： We present an approach for initiating and tracing ultrafast electron dynamics in core-excited atoms, molecules, and solids. The approach is based on stimulated resonant inelastic x-ray scattering induced by a single, chirped, broadband XUV or x-ray pulse. A first interaction with this pulse prepares a core-excited state wave packet by resonant core-excitation. A second interaction with the pulse at a later time induces the transition to valence-excited states, which is associated with stimulated emission. The preparation of the core-excited wave packet and the transition from the core-excited states to the valence-excited states occur at distinct chirp-dependent times. As a consequence, the stimulated emission carries information about the time evolution of the core-excited state wave packet.
关键词： XUV pulses,x-ray pulses,core-excited states,ultrafast electron dynamics,chirped pulses,stimulated resonant inelastic x-ray scattering
更新于2025-09-19 17:15:36