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Register a new userX-Ray Thomson scattering without the Chihara decomposition
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X-Ray Thomson Scattering (XRTS) is an important experimental technique used to measure the temperature, ionization state, structure, and density of warm dense matter (WDM). The fundamental property probed in these experiments is the electronic dynamic structure factor (DSF). In most models, this is decomposed into three terms [Chihara, J. Phys. F: Metal Phys. {bf 17}, 295 (1987)] representing the response of tightly bound, loosely bound, and free electrons. Accompanying this decomposition is the classification of electrons as either bound or free, which is useful for gapped and cold systems but becomes increasingly questionable as temperatures and pressures increase into the WDM regime. In this work we provide unambiguous first principles calculations of the dynamic structure factor of warm dense beryllium, independent of the Chihara form, by treating bound and free states under a single formalism. The computational approach is real-time finite-temperature time-dependent density functional theory (TDDFT) being applied here for the first time to WDM. We compare results from TDDFT to Chihara-based calculations for experimentally relevant conditions in shock-compressed beryllium.
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Non-destructive determination of lithium distribution in a working battery is key for addressing both efficiency and safety issues. Although various techniques have been developed to map the lithium distribution in electrodes, these methods are mostly applicable to test cells. Here we propose the use of high-energy x-ray Compton scattering spectroscopy to measure the local lithium concentration in closed electrochemical cells. A combination of experimental measurements and parallel first-principles computations is used to show that the shape parameter S of the Compton profile is linearly proportional to lithium concentration and thus provides a viable descriptor for this important quantity. The merits and applicability of our method are demonstrated with illustrative examples of LixMn2O4 cathodes and a working commercial lithium coin battery CR2032.
For the last decade numerous researchers have been trying to develop experimental techniques to use X-ray Thomson scattering as a method to measure the temperature, electron density, and ionization state of high energy density plasmas such as those used in inertial confinement fusion. With the advent of the X-ray free electron laser (X-FEL) at the SLAC Linac Coherent Light Source (LCLS) we now have such a source available in the keV regime. One challenge with X-ray Thomson scattering experiments is understanding how to model the scattering for partially ionized plasmas. Most Thomson scattering codes used to model experimental data greatly simplify or neglect the contributions of the bound electrons to the scattered intensity. In this work we take the existing models of Thomson scattering that include elastic ion-ion scattering and the electron-electron plasmon scattering and add the contribution of the bound electrons in the partially ionized plasmas. Except for hydrogen plasmas almost every plasma that is studied today has bound electrons and it is important to understand their contribution to the Thomson scattering, especially as new X-ray sources such as the X-FEL will allow us to study much higher Z plasmas. Currently most experiments have looked at hydrogen or beryllium. We will first look at the bound electron contributions to beryllium by analysing existing experimental data. We then consider several higher Z materials such as Cr and predict the existence of additional peaks in the scattering spectrum that requires new computational tools to understand. For a Sn plasma we show that the bound contributions changes the shape of the scattered spectrum in a way that would change the plasma temperature and density inferred by the experiment.
Chemical interaction and changes in local electronic structure of Cr, Fe, Co, Ni and Cu transition metals (TMs) upon formation of an $Al_{8}Co_{17}Cr_{17}Cu_{8}Fe_{17}Ni_{33}$ compositionally complex alloy (CCA) have been studied by X-ray absorption spectroscopy and X-ray photoelectron spectroscopy. It was found that upon CCA formation, occupancy of the Cr, Co and Ni 3d states changes and the maximum of the occupied and empty Ni 3d states density shifts away from Fermi level ($E_f$) by 0.5 and 0.6 eV, respectively, whereas the Cr 3d empty states maximum shifts towards $E_f$ by 0.3 eV, compared to the corresponding pure metals. The absence of significant charge transfer between the elements was established, pointing to the balancing of the 3d states occupancy change by involvement of delocalized 4s and 4p states into the charge redistribution. Despite the expected formation of strong Al-TMs covalent bonds, the Al role in the transformation of the TMs 3d electronic states is negligible. The work demonstrates a decisive role of Cr in the Ni local electronic structure transformation and suggests formation of directional Ni-Cr bonds with covalent character. These findings can be helpful for tuning deformation properties and phase stability of the CCA.
Resonance anomalous surface x-ray scattering (RASXS) technique was applied to electrochemical interface studies. It was used to determine the chemical states of electrochemically formed anodic oxide monolayers on platinum surface. It is shown that RASXS exhibits strong polarization dependence when the surface is significantly modified. The polarization dependence is demonstrated for three examples; anodic oxide formation, sulfate adsorption, and CO adsorption on platinum surfaces. s- and p- polarization RASXS data were simulated with the latest version of ab initio multiple scattering calculations (FEFF8.2). Elementary theoretical considerations are also presented for the origin of the polarization dependence in RASXS.
An outstanding challenge of theoretical electronic structure is the description of van der Waals (vdW) interactions in molecules and solids. Renewed interest in resolving this is in part motivated by the technological promise of layered systems including graphite, transition metal dichalcogenides, and more recently, black phosphorus, in which the interlayer interaction is widely believed to be dominated by these types of forces. We report a series of quantum Monte Carlo (QMC) calculations for bulk black phosphorus and related few-layer phosphorene, which elucidate the nature of the forces that bind these systems and provide benchmark data for the energetics of these systems. We find a significant charge redistribution due to the interaction between electrons on adjacent layers. Comparison to density functional theory (DFT) calculations indicate not only wide variability even among different vdW corrected functionals, but the failure of these functionals to capture the trend of reorganization predicted by QMC. The delicate interplay of steric and dispersive forces between layers indicate that few-layer phosphorene presents an unexpected challenge for the development of vdW corrected DFT.
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