arXiv subjects

Simo Huotari

Publications and source records attributed to Simo Huotari.

At least 19 recordsLinked to original sources

arXiv2024

The Heisenberg-RIXS instrument at the European XFEL

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.

cond-mat.str-el↗

arXiv2023

Inner product regularized multi-energy X-ray tomography for material decomposition

Multi-energy X-ray tomography is studied for decomposing three materials using three X-ray energies and a classical energy-integrating detector. A novel regularization term comprises inner products between the material distribution functions, penalizing any overlap of different materials. The method is tested on real data measured of a phantom embedded with Na$_2$SeO$_3$, Na$_2$SeO$_4$, and elemental selenium. It is found that the two-dimensional distributions of selenium in different oxidation states can be mapped and distinguished from each other with the new algorithm. The results have applications in material science, chemistry, biology and medicine.

cond-mat.mtrl-sci↗

arXiv2023

Paramagnon dispersion and damping in doped Na$_{x}$Ca$_{2-x}$CuO$_2$Cl$_2$

Using Resonant Inelastic X-ray Scattering, we measure the paramagnon dispersion and damping of undoped, antiferromagnetic Ca$_2$CuO$_2$Cl$_2$ as well as doped, superconducting Na$_{x}$Ca$_{2-x}$CuO$_2$Cl$_2$. Our estimation of the spin-exchange parameter and width of the paramagnon peak at the zone boundary $X=(0.5,0)$ confirms that no simple relation can be drawn between these parameters and the critical temperature $T_\mathrm{c}$. Consistently with other cuprate compounds, we show that upon doping there is a slight softening at $(0.25,0)$, but not at the zone boundary $X$. In combination with these measurements we perform calculations of the dynamical spin structure factor of the one-band Hubbard model using cluster dynamical mean-field theory. The calculations are in excellent agreement with the experiment in the undoped case, both in terms of energy position and width. While the increase in width is also captured upon doping, the dynamical spin structure factor shows a sizable softening at $X$, which provides insightful information on the length-scale of the spin fluctuations in doped cuprates.

cond-mat.supr-con↗

arXiv2022

Monochromatic computed tomography using laboratory-scale setup: proof-of-concept

In this article, we demonstrate the viability of highly monochromatic full-field X-ray absorption near edge structure based tomography using a laboratory-scale Johann-type X-ray absorption spectrometer based on a conventional X-ray tube source. In this proof-of-concept, by using a phantom embedded with elemental Se, Na$_2$SeO$_3$, and Na$_2$SeO$_4$, we show that the three-dimensional distributions of Se in different oxidation states can be mapped and distinguished from the phantom matrix and each other with absorption edge contrast tomography. The presented method allows for volumetric analyses of chemical speciation in mm-scale samples using low-brilliance X-ray sources, and represents a new analytic tool for materials engineering and research in many fields including biology and chemistry.

physics.ins-det↗

arXiv2021

Redox oscillations in 18650-type lithium-ion cell revealed by in operando Compton scattering imaging

Compton scattering imaging using high-energy synchrotron x-rays allows the visualization of the spatio-temporal lithiation state in lithium-ion batteries probed in-operando. Here, we apply this imaging technique to the commercial 18650-type cylindrical lithium-ion battery. Our analysis of the lineshapes of the Compton scattering spectra taken from different electrode layers reveals the emergence of inhomogeneous lithiation patterns during the charge-discharge cycles. Moreover, these patterns exhibit oscillations in time where the dominant period corresponds to the time scale of the charging curve.

physics.app-ph↗

arXiv2021

Towards novel probes for valence charges via X-ray optical wave mixing

We present a combined theoretical and experimental study of X-ray optical wave mixing. This class of nonlinear phenomena combines the strengths of spectroscopic techniques from the optical domain, with the high-resolution capabilities of X-rays. In particular, the spectroscopic sensitivity of these phenomena can be exploited to selectively probe valence dynamics. Specifically, we focus on the effect of X-ray parametric down-conversion. We present a theoretical description of the process, from which we deduce the observable nonlinear response of valence charges. Subsequently, we simulate scattering patterns for realistic conditions and identify characteristic signatures of the nonlinear conversion. For the observation of this signature, we present a dedicated experimental setup and results of a detailed investigation. However, we do not find evidence of the nonlinear effect. This finding stands in strong contradiction to previous claims of proof-of-principle demonstrations. Nevertheless, we are optimistic to employ related X-ray optical wave mixing processes on the basis of the methods presented here for probing valence dynamics in the future.

physics.optics↗

arXiv2020

General method to calculate the elastic deformation and X-ray diffraction properties of bent crystal wafers

Curved single crystals are widely employed in spectrometer designs in the hard X-ray regime. Due to their large solid angle coverage and focusing properties, toroidally bent crystals are extremely useful in applications where the output of photons is low. Spherically bent crystals, a subgroup of toroidally bent crystals, particularly have found their way in many instruments at synchtrotrons and free electron laser lightsource end-stations but also in the re-emerging field of high-resolution laboratory-scale X-ray spectroscopy. A solid theoretical understanding of the diffraction properties of such crystals is essential when aiming for optimal spectrometer performance. In this work, we present a general method to calculate the internal stress and strain fields of toroidally bent crystals and how to apply it to predict their diffraction properties. Solutions are derived and discussed for circular and rectangular spherically bent wafers due to their prevalence in contemporary instrumentation.

physics.ins-det↗

arXiv2020

Sparse dynamic tomography. A shearlet-based approach for iodine perfusion in plant stems

In this paper we propose a motion-aware variational approach to reconstruct moving objects from sparse dynamic data. The motivation of this work stems from X-ray imaging of plants perfused with a liquid contrast agent, aimed at increasing the contrast of the images and studying the phloem transport in plants over time. The key idea of our approach is to deploy 3D shearlets as a space-temporal prior, treating time as the third dimension. The rationale behind this model is that a continuous evolution of a cartoon-like object is well suited for the use of 3D shearlets. We provide a basic mathematical analysis of the variational model for the image reconstruction. The numerical minimization is carried out with primal-dual scheme coupled with an automated choice of regularization parameter. We test our model on different measurement setups: a simulated phantom especially designed to resemble a plant stem, with spreading points to simulate a spreading contrast agent; a measured agarose gel phantom to demonstrate iodide diffusion and geometry prior to imaging living sample; a measured living tree grown \textit{in vitro} and perfused with a liquid sugar-iodine-mix. The results, compared against a 2D static model, show that our approach provides reconstructions that capture well the time dynamic of the contrast agent onset and are encouraging to develop microCT as a tool to study phloem transport using iodine tracer.

eess.IV↗

arXiv2018

Johann-type laboratory-scale X-ray absorption spectrometer with versatile detection modes

We present a low-cost laboratory X-ray absorption spectrometer that uses a conventional X-ray tube source and bent Johann-type crystal monochromators. The instrument is designed for XAS studies in the 4-20 keV range which covers most K edges of 3d transition metals and L edges of 5d transition metals and actinides. The energy resolution is typically in the range of 1-5 eV at 10 keV depending on the crystal analyser and the Bragg angle. Measurements can be performed in transmission, fluorescence, and imaging modes. Due to its simple and modular design, the spectrometer can be modified to accommodate additional equipment and complex sample environments required for e.g. in situ studies. A showcase of various applications is presented.

physics.ins-det↗

arXiv2018

The isotropic Compton profile difference across the phase transition of VO$_2$

We studied the isotropic Compton profile of the prototypical oxide VO$_2$ across the temperature induced electronic and structural phase transition at T$_C$ $\approx$ 340 K. We show that the phase transition leaves an observable signal, which facilitates Compton scattering studies of electronic structure and phase transitions in complex solids in powder form. We compare the experimental results with density functional theory calculations and find agreement in the shape of the difference profile, although the amplitude of the observed features is overestimated. The origin of the disagreement is discussed and we argue that it mainly originates mostly correlation effects beyond our current calculations and possibly to some extent, from thermal motion.

cond-mat.str-el↗

arXiv2016

Tomographic X-ray data of a lotus root filled with attenuating objects

This is the documentation of the tomographic X-ray data of a lotus root, filled with four different attenuating objects, of different sizes. Data are available at www.fips.fi/dataset.php, and can be freely used for scientific purposes with appropriate references to them, and to this document in http://arxiv.org/arXiv. The data set consists of (1) the X-ray sinogram of a single 2D slice of the lotus root with two different resolutions and (2) the corresponding measurement matrices modeling the linear operation of the X-ray transform. Each of these sinograms was obtained from a measured 360-projection fan-beam sinogram by down-sampling and taking logarithms. The original (measured) sinogram is also provided in its original form and resolution.

physics.data-an↗

arXiv2016

Electron-energy-loss and time-dependent density functional theory study on the plasmon dispersion in 2H-NbS2

We examine the experimental and theoretical electron-energy loss spectra in 2$H$-Cu$_{0.2}$NbS$_2$ and find that the 1 eV plasmon in this material does not exhibit the regular positive quadratic plasmon dispersion that would be expected for a normal broad-parabolic-band system. Instead we find a nearly non-dispersing plasmon in the momentum-transfer range $q<0.35$ \AA$^{-1}$. We argue that for a stoichiometric pure 2$H$-NbS$_2$ the dispersion relation is expected to have a negative slope as is the case for other transition-metal dichalcogenides. The presence of Cu impurities, required to stabilize the crystal growth, tends to shift the negative plasmon dispersion into a positive one, but the doping level in the current system is small enough to result in a nearly-non-dispersing plasmon. We conclude that a negative-slope plasmon dispersion is not connected with the existence of a charge-density-wave order in transition metal dichalcogenides.

cond-mat.str-el↗

arXiv2016

A computationally efficient method to solve the Takagi-Taupin equations for a large deformed crystal

We present a treatise on solving the Takagi-Taupin equations in the case of a strain field with an additional, spatially slowly varying component (owing to \emph{e.g.}~heat expansion or angular compression). We show that the presence of such a component in a typical case merely shifts the reflectivity curve as a function of wavelength or incidence angle, while having a negligible effect on its shape. On the basis of the derived result, we develop a computationally efficient method to calculate the reflectivity curve of a large deformed crystal. The validity of the method is demonstrated by comparing computed reflectivity curves with experimental ones for bent silicon wafers. A good agreement is observed.

physics.optics↗

arXiv2015

Resonant X-ray Emission Spectroscopy With a Standing Wave Excitation

The Borrmann effect is the anomalous transmission of x rays in perfect crystals under diffraction conditions. It arises from the interference of the incident and diffracted waves, which creates a standing wave with nodes at strongly absorbing atoms. Dipolar absorption of x rays is thus diminished, which makes the crystal nearly transparent for certain x-ray wave vectors. Indeed, a relative enhancement of electric quadrupole absorption via the Borrmann effect has been demonstrated recently. Here we show that the Borrmann effect has a significantly larger impact on resonant x-ray emission than is observable in x-ray absorption. Emission from a dipole forbidden intermediate state may even dominate the corresponding x-ray spectra. Our work extends the domain of x-ray standing wave methods to resonant x-ray emission spectroscopy and provides means for novel spectroscopic experiments in d- and f-electron systems.

cond-mat.mtrl-sci↗

arXiv2015

Exciton energy-momentum map of hexagonal boron nitride

Understanding and controlling the way excitons propagate in solids is a key for tailoring materials with improved optoelectronic properties. A fundamental step in this direction is the determination of the exciton energy-momentum dispersion. Here, thanks to the solution of the parameter-free Bethe- Salpeter equation (BSE), we draw and explain the exciton energy-momentum map of hexagonal boron nitride (h-BN) in the first three Brillouin zones. We show that h-BN displays strong excitonic effects not only in the optical spectra at vanishing momentum $\mathbf{q}$, as previously reported, but also at large $\mathbf{q}$. We validate our theoretical predictions by assessing the calculated exciton map by means of an inelastic x-ray scattering (IXS) experiment. Moreover, we solve the discrepancies between previous experimental data and calculations, proving then that the BSE is highly accurate through the whole momentum range. Therefore, these results put forward the combination BSE and IXS as the tool of choice for addressing the exciton dynamics in complex materials.

cond-mat.mtrl-sci↗

arXiv2013

Temperature dependence of crystal field excitations in CuO

We report a study on the temperature dependence of the charge-neutral crystal field (dd) excitations in cupric oxide, using nonresonant inelastic x-ray scattering (IXS) spectroscopy. Thanks to a very high energy resolution (60 meV), we observe thermal effects on the dd excitation spectrum fine structure between temperatures of 10-320 K. With an increasing temperature, the spectra broaden considerably. We assign the temperature dependence of the dd excitations to the relatively large electron-phonon coupling.

cond-mat.str-el↗

arXiv2012

Momentum distribution and Compton profile by the ab initio GW approximation

We present two possible approaches to calculate the momentum distribution n(p) and the Compton profile within the framework of the ab initio GW approximation on the self-energy. The approaches are based on integration of the Green's function along either the real or the imaginary axes. Examples will be presented on the jellium model and on real bulk sodium. Advantages and drawbacks of both methods are discussed in comparison with accurate quantum Monte Carlo (QMC) calculations and x-ray Compton scattering experiments. We illustrate the effect of many-body correlations and disentangle them from band-structure and anisotropy effects by a comparison with density functional theory in the local density approximation. Our results suggest the use of G0W0 momentum distributions as reference for future experiments and theory developments.

cond-mat.other↗

arXiv2010

Screening in YBCO at large wave vectors

We present experimental inelastic x-ray scattering (IXS) and ab initio time-dependent density-functional-theory (TDDFT) studies of YBa2Cu3O7-δ. The response of the low-lying Ba 5p and Y 4p core electrons is shown to interact strongly with the Cu 3d and O 2p excitations, with important consequences on screening. The agreement between IXS and TDDFT results is excellent, apart from a new type of excitations, mainly related to loosely bound Ba electrons and significantly affected by correlations. This points to correlation mechanisms not fully described by TDDFT that might have a role in giving rise to antiscreening.

cond-mat.supr-con↗