| 1. |
- Abrikosov, Igor, 1965-, et al.
(författare)
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Local environment effects in random metallic alloys
- 2005. - 1
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Ingår i: The Science of Complex Alloy Phases. - USA : TMS. - 087339593X - 9780873395939 ; , s. 87-108
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Bokkapitel (övrigt vetenskapligt/konstnärligt)abstract
- This book is published in honor of the 2005 Hume-Rothery Award Recipient, Uichiro Mizutani. It emphasizes both theoretical and experimental aspects of electronic, structural, and thermodynamic properties of complex alloy phases. Leading experts provide an assessment of our current understanding of the structural properties of complex materials, including quasicrystalline and amorphous alloys. Special emphasis is placed on our understanding of why nature is able to stabilize complex atomic arrangements and on recent results related to structurally complex alloy phases. These topics, in the spirit of the work carried out by U. Mizutani, constitute the main theme of the book
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| 2. |
- Belonoshko, Anatoly, et al.
(författare)
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Elastic properties of body-centered cubic iron in Earth's inner core
- 2022
-
Ingår i: Physical Review B. - : American Physical Society (APS). - 2469-9950 .- 2469-9969. ; 105:18
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Tidskriftsartikel (refereegranskat)abstract
- The solid Earth's inner core (IC) is a sphere with a radius of about 1300 km in the center of the Earth. The information about the IC comes mainly from seismic studies. The composition of the IC is obtained by matching the seismic data and properties of candidate phases subjected to high pressure (P) and temperature (T). The close match between the density of the IC and iron suggests that the main constituent of the IC is iron. However, the stable phase of iron is still a subject of debate. One such iron phase, the body-centered cubic phase (bcc), is dynamically unstable at pressures of the IC (330-364 GPa) and low T but gets stabilized at high T characteristic of the IC (5000-7000 K). So far, ab initio molecular dynamics (AIMD) studies attempted to compute the bcc elastic properties for a small (order of 102) number of atoms. The mechanism of the bcc stabilization cannot be enabled in such cells and that has led to erroneous results. Here we apply AIMD to compute elastic moduli and sound velocities of the Fe bcc phase for a 2000 Fe atom computational cell, which is a cell of unprecedented size for ab initio calculations of iron. Unlike in previous ab initio calculations, both the longitudinal and the shear sound velocities of the Fe bcc phase closely match the properties of the IC material at P = 360 GPa and T = 6600 K, likely the PT conditions in the IC. The calculated density of the bcc iron at these PT conditions is just 3% higher than the density of the IC material according to the Preliminary Earth Model. This suggests that the widely assumed amount of light elements in the IC may need a reconsideration. The anisotropy of the bcc phase is an exact match to the most recent seismic studies.
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| 3. |
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| 4. |
- Eriksson, Peter, et al.
(författare)
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Cerium oxide nanoparticles with antioxidant capabilities and gadolinium integration for MRI contrast enhancement
- 2018
-
Ingår i: Scientific Reports. - : Nature Publishing Group. - 2045-2322. ; 8
-
Tidskriftsartikel (refereegranskat)abstract
- The chelating gadolinium-complex is routinely used as magnetic resonance imaging (MRI) -contrast enhancer. However, several safety issues have recently been reported by FDA and PRAC. There is an urgent need for the next generation of safer MRI-contrast enhancers, with improved local contrast and targeting capabilities. Cerium oxide nanoparticles (CeNPs) are designed with fractions of up to 50% gadolinium to utilize the superior MRI-contrast properties of gadolinium. CeNPs are well-tolerated in vivo and have redox properties making them suitable for biomedical applications, for example scavenging purposes on the tissue-and cellular level and during tumor treatment to reduce in vivo inflammatory processes. Our near edge X-ray absorption fine structure (NEXAFS) studies show that implementation of gadolinium changes the initial co-existence of oxidation states Ce3+ and Ce4+ of cerium, thereby affecting the scavenging properties of the nanoparticles. Based on ab initio electronic structure calculations, we describe the most prominent spectral features for the respective oxidation states. The as-prepared gadolinium-implemented CeNPs are 3-5 nm in size, have r(1)-relaxivities between 7-13 mM(-1) s(-1) and show clear antioxidative properties, all of which means they are promising theranostic agents for use in future biomedical applications.
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| 5. |
- Fallqvist, Amie, et al.
(författare)
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Evidence for B1-cubic SiNx by Aberration-Corrected Analytical STEM
-
Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- The crystal structure of epitaxially stabilized SiNx layers on TiN(001) was investigated by analytical aberration corrected electron microscopy. Atomically resolved images of the structure, which were acquired by scanning transmission electron microscopy using high angle annular dark field and annular bright field detectors, are used to identify the B1-cubic structure of SiNx. To corroborate the acquired images, image simulations were performed using candidate structures. Complementary to imaging, spatially resolved electron energy loss spectroscopy of the epitaxial SiNx layers was performed to acquire the symmetry specific nitrogen near edge fine-structure. Finally, full potential calculations performed to determine the near edge structure from candidate crystal structures confirms the existence of B1-cubic SiNx.
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| 6. |
- Fallqvist, Amie, et al.
(författare)
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Resolving the debated atomic structure of the metastable cubic SiNx tissue phase in nanocomposites with TiN
- 2018
-
Ingår i: Physical Review Materials. - : American Physical Society. - 2475-9953. ; 2:9
-
Tidskriftsartikel (refereegranskat)abstract
- The TiN/SiNx nanocomposite and nanolaminate systems are the archetype for super if not ultrahard materials. Yet, the nature of the SiNx tissue phase is debated. Here, we show by atomically resolved electron microscopy methods that SiNx is epitaxially stabilized in a NaCl structure on the adjacent TiN(001) surfaces. Additionally, electron energy loss spectroscopy, supported by first-principles density functional theory calculations infer that SiNx hosts Si vacancies.
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| 7. |
- Granroth, Sari, et al.
(författare)
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Investigation of interface properties of Ni/Cu multilayers by high kinetic energy photoelectron spectroscopy
- 2009
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Ingår i: Physical Review B (Condensed Matter and Materials Physics). - 1098-0121 .- 1550-235X. ; 80:9
-
Tidskriftsartikel (refereegranskat)abstract
- High kinetic-energy photoelectron spectroscopy (HIKE) or hard x-ray photoelectron spectroscopy has been used to investigate the alloying of Ni/Cu (100) multilayers. Relative intensities of the corelevels and their chemical shifts derived from binding energy changes are shown to give precise information on physicochemical properties and quality of the buried layers. Interface roughening, including kinetic properties such as the rate of alloying, and temperature effects on the processes can be analyzed quantitatively. Using HIKE, we have been able to precisely follow the deterioration of the multilayer structure at the atomic scale and observe the diffusion of the capping layer into the multilayer structure which in turn is found to lead to a segregation in the ternary system. This is of great importance for future research on multilayered systems of this kind. Our experimental data are supplemented by first-principles theoretical calculations of the core-level shifts for a ternary alloy to allow for modeling of the influence of capping materials on the chemical shifts.
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| 8. |
- Granroth, Sari, et al.
(författare)
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Understanding interface properties from high kinetic energy photoelectron spectroscopy and first principles theory
- 2011
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Ingår i: Journal of Electron Spectroscopy and Related Phenomena. - : Elsevier BV. - 0368-2048 .- 1873-2526. ; 183:1-3, s. 80-93
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Forskningsöversikt (refereegranskat)abstract
- Advances in instrumentation regarding 3rd generation synchrotron light sources and electron spectrometers has enabled the field of high kinetic energy photoelectron spectroscopy (HIKE) (also often denoted hard X-ray photoelectron spectroscopy (HX-PES or HAXPES)). Over the last years, the amount of investigations that relies on the HIKE method has increased dramatically and can arguably be said to have given a rebirth of the interest in photoelectron spectroscopy in many areas. It is in particular the much increased mean free path at higher kinetic energies in combination with the elemental selectivity of the core level spectroscopies in general that has lead to this fact, as it makes it possible to investigate the electronic structure of materials with a substantially reduced surface sensitivity. In this review we demonstrate how HIKE can be used to investigate the interface properties in multilayer systems. Relative intensities of the core level photoelectron peaks and their chemical shifts derived from binding energy changes are found to give precise information on physico-chemical properties and quality of the buried layers. Interface roughening, including kinetic properties such as the rate of alloying, and temperature effects on the processes can be analyzed quantitatively. We will also provide an outline of the theoretical framework that is used to support the interpretation of data. We provide examples from our own investigations of multilayer systems which comprises both systems of more model character and a multilayer system very close to real applications in devices that are considered to be viable alternative to the present read head technology. The experimental data presented in this review is exclusively recorded at the BESSY-II synchrotron at the Helmholtz-Zentrum Berlin fur-Materialien und Energie. This HIKE facility is placed at the bending magnet beamline KMC-1, which makes it different from several other facilities which relies on undulators as the source. We will therefore also briefly describe some of the salient design features of this facility.
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| 9. |
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| 10. |
- Göransson Asker, Christian, et al.
(författare)
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Numerical investigation of the validity of the Slater-Janak transition-state model in metallic systems
- 2005
-
Ingår i: Physical Review B. Condensed Matter and Materials Physics. - 1098-0121 .- 1550-235X. ; 72:13
-
Tidskriftsartikel (refereegranskat)abstract
- According to the so-called Janak’s theorem, the eigenstates of the Kohn-Sham Hamiltonian are given by the derivative of the total energy with respect to the occupation numbers of the corresponding one-electron states. The linear dependence of the Kohn-Sham eigenvalues on the occupation numbers is often assumed in order to use the Janak’s theorem in applications, for instance, in calculations of the core-level shifts in materials by means of the Slater-Janak transition state model. In this work first-principles density-functional theory calculations using noninteger occupation numbers for different core states in 24 different random alloy systems were carried out in order to verify the assumptions of linearity. It is found that, to a first approximation, the Kohn-Sham eigenvalues show a linear behavior as a function of the occupation numbers. However, it is also found that deviations from linearity have observable effects on the core-level shifts for some systems. A way to reduce the error with minimal increase of computational efforts is suggested.
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| 11. |
- Magnuson, Martin, 1965-, et al.
(författare)
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Interface bonding of Zr1−xAlxN nanocomposites investigated by x-ray spectroscopies and first principles calculations
- 2020
-
Ingår i: Physical Review Research. - College Park, MD, United States : American Physical Society. - 2643-1564. ; 2:1
-
Tidskriftsartikel (refereegranskat)abstract
- The electronic structure, chemical bonding, and interface component in ZrN-AlN nanocomposites formed byphase separation during thin film deposition of metastable Zr1−xAlxN (x = 0.0, 0.12, 0.26, 0.40) are investigatedby resonant inelastic x-ray scattering, x-ray emission, and x-ray absorption spectroscopy and compared to firstprinciples calculations including transitions between orbital angular momentum final states. The experimentalspectra are compared with different interface-slab model systems using first principles all-electron full-potentialcalculations where the core states are treated fully relativistically. As shown in this work, the bulk sensitivity andelement selectivity of x-ray spectroscopy enables one to probe the symmetry and orbital directions at interfacesbetween cubic and hexagonal crystals. We show how the electronic structure develops from local octahedralbond symmetry of cubic ZrN that distorts for increasing Al content into more complex bonding. This results inthree different kinds of bonding originating from semicoherent interfaces with segregated ZrN and lamellar AlNnanocrystalline precipitates. An increasing chemical shift and charge transfer between the elements takes placewith increasing Al content and affects the bond strength and increases resistivity.
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| 12. |
- Marten, Tobias, 1979-, et al.
(författare)
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Ab initio study of disorder broadening of core photoemission spectra in random Cu-Pd and Ag-Pd alloys
- 2005
-
Ingår i: Physical Review B. Condensed Matter and Materials Physics. - 1098-0121 .- 1550-235X. ; 72:5
-
Tidskriftsartikel (refereegranskat)abstract
- A first-principles study of the effect of local environment on the electronic structure of random face-centered cubic Ag-Pd and Cu-Pd alloys is presented. The core-level shift for each atom in the equiatomic alloys is calculated and compared to experimental data. It is shown how the initial-state and final-state distributions contribute to the total broadening. We find that the initial-state and the final-state contributions together increase the broadening for the investigated core levels in Cu and Ag, whereas they cancel each other to a large degree for Pd. We also demonstrated how local lattice relaxations influence the binding energy shift. We find that relaxation does not influence the average shift, though it is able to affect the broadening of the simulated x-ray photoelectron spectroscopy spectra. © 2005 The American Physical Society.
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| 13. |
- Mizoguchi, T., et al.
(författare)
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Excitonic, vibrational, and van der Waals interactions in electron energy loss spectroscopy
- 2017
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Ingår i: Ultramicroscopy. - : ELSEVIER SCIENCE BV. - 0304-3991 .- 1879-2723. ; 180, s. 93-103
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Tidskriftsartikel (refereegranskat)abstract
- The pioneer, Ondrej L. Krivanek, and his collaborators have opened up many frontiers for the electron energy loss spectroscopy (EELS), and they have demonstrated new potentials of the EELS method for investigating materials. Here, inspired by those achievements, we show further potentials of EELS based on the results of theoretical calculations, that is excitonic and van der Waals (vdW) interactions, as well as vibrational information of materials. Concerning the excitonic interactions, we highlight the importance of the two-particle calculation to reproduce the low energy-loss near-edge structure (ELNES), the Na-L-2,L-3 edge of Nal and the Li-K edge of LiCI and LiFePO4. Furthermore, an unusually strong excitonic interaction at the O-K edge of perovskite oxides, SrTiO3 and LaAlO3, is shown. The effect of the vdW interaction in the ELNES is also investigated, and we observe that the magnitude of the vdW effect is approximately 0.1 eV in the case of the ELNES from a solid and liquid, whereas its effect is almost negligible in the case of the ELNES from the gaseous phase owing to the long inter-molecular distance. In addition to the static information, the influence of the dynamic behavior of atoms in materials to EELS is also investigated. We show that measurements of the infrared spectrum are possible by using a modern monochromator system. Furthermore, an estimation of the atomic vibration in core-loss ELNES is also presented. We show the acquisition of vibrational information using the ELNES of liquid methanol and acetic acid, solid Al2O3, and oxygen gas. (C) 2017 Elsevier B.V. All rights reserved.
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| 14. |
- Monteseguro, V, et al.
(författare)
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Phase stability and electronic structure of iridium metal at the megabar range
- 2019
-
Ingår i: Scientific Reports. - : Nature Publishing Group. - 2045-2322. ; 9
-
Tidskriftsartikel (refereegranskat)abstract
- The 5d transition metals have attracted specific interest for high-pressure studies due to their extraordinary stability and intriguing electronic properties. In particular, iridium metal has been proposed to exhibit a recently discovered pressure-induced electronic transition, the so-called core-level crossing transition at the lowest pressure among all the 5d transition metals. Here, we report an experimental structural characterization of iridium by x-ray probes sensitive to both long- and short-range order in matter. Synchrotron-based powder x-ray diffraction results highlight a large stability range (up to 1.4 Mbar) of the low-pressure phase. The compressibility behaviour was characterized by an accurate determination of the pressure-volume equation of state, with a bulk modulus of 339(3) GPa and its derivative of 5.3(1). X-ray absorption spectroscopy, which probes the local structure and the empty density of electronic states above the Fermi level, was also utilized. The remarkable agreement observed between experimental and calculated spectra validates the reliability of theoretical predictions of the pressure dependence of the electronic structure of iridium in the studied interval of compressions.
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| 15. |
- Mosyagin, Igor, et al.
(författare)
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Highly Efficient Free Energy Calculations of the Fe Equation of State Using Temperature-Dependent Effective Potential Method
- 2016
-
Ingår i: Journal of Physical Chemistry A. - : American Chemical Society (ACS). - 1089-5639 .- 1520-5215. ; 120:43, s. 8761-8768
-
Tidskriftsartikel (refereegranskat)abstract
- Free energy calculations at finite temperature based on ab initio molecular dynamics (AIMD) simulations have become possible, but they are still highly computationally demanding. Besides, achieving simultaneously high accuracy of the calculated results and efficiency of the computational algorithm is still a challenge. In this work we describe an efficient algorithm to determine accurate free energies of solids in simulations using the recently proposed temperature-dependent effective potential method (TDEP). We provide a detailed analysis of numerical approximations employed in the TDEP algorithm. We show that for a model system considered in this work, hcp Fe, the obtained thermal equation of state at 2000 K is in excellent agreement with the results of standard calculations within the quasiharmonic approximation.
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| 16. |
- Olovsson, Weine, et al.
(författare)
-
Core-level shifts in complex metallic systems from first principle
- 2006
-
Ingår i: Physica status solidi. B, Basic research. - : Wiley. - 0370-1972 .- 1521-3951. ; 243:11, s. 2447-2464
-
Tidskriftsartikel (refereegranskat)abstract
- We show that core-level binding energy shifts (CLS) can be reliably calculated within density functional theory. The scheme includes both the initial (electron energy eigenvalue) as well as final state (relaxation due to core-hole screening) effects in the same framework. The results include CLS as a function of composition in substitutional random bulk and surface alloys. Sensitivity of the CLS to the local chemical environment in the bulk and at the surface is demonstrated. A possibility to use the CLS for structural determination is discussed. Finally, an extension of the model is made for Auger kinetic energy shift calculations.
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| 17. |
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| 18. |
- Olovsson, Weine, et al.
(författare)
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First principle calculations of core-level binding energy and Auger kinetic energy shifts in metallic solids
- 2010
-
Ingår i: Journal of Electron Spectroscopy and Related Phenomena. - : Elsevier BV. - 0368-2048 .- 1873-2526. ; 178-179:C, s. 88-99
-
Tidskriftsartikel (refereegranskat)abstract
- We present a brief overview of recent theoretical studies of the core-level binding energy shift (CLS) in solid metallic materials. The focus is on first principles calculations using the complete screening picture, which incorporates the initial (ground state) and final (core-ionized) state contributions of the electron photoemission process in X-ray photoelectron spectroscopy (XPS), all within density functional theory (DFT). Considering substitutionally disordered binary alloys, we demonstrate that on the one hand CLS depend on average conditions, such as volume and overall composition, while on the other hand they are sensitive to the specific local atomic environment. The possibility of employing layer resolved shifts as a tool for characterizing interface quality in fully embedded thin films is also discussed, with examples for CuNi systems. An extension of the complete screening picture to core-core-core Auger transitions is given, and new results for the influence of local environment effects on Auger kinetic energy shifts in fcc AgPd are presented.
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| 19. |
- Olovsson, Weine, 1975-
(författare)
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Influence of Global Composition and Local Environment on the Spectroscopic and Magnetic Properties of Metallic Alloys
- 2005
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Theoretical investigations of spectroscopic and magnetic properties of metallic systems in the bulk, as well as in nanostructured materials, have been performed within the density functional theory. The major part of the present work studies the differences between binding energies of electrons tightly bound to the atoms, the so-called core electrons (in contrast with the valence electrons), that is, core-level binding energy shift (CLS). By comparison between corresponding elemental core-levels for atoms situated in different chemical environments we obtain fundamental understanding of bonding properties of materials. The method of choice was the complete screening picture, which includes initial and final state effects on the same footing. The usefulness of CLS stems from that it is sensitive to differences in the chemical environment of an atom, which can be affected on one hand by the global composition of e.g. disordered materials, surfaces and interfaces, and on the other hand by the very local environment around an atom. Here CLSs have been obtained for both components in the fcc random alloys AgPd, CuPd, CuNi, CuPt, CuAu, PdAu, NiPd and NiPt. Moreover the model was extended to the Auger kinetic energy shift for the LMM Auger transition in AgPd alloys. Studies were also applied to the near surface and interface regions of PdMn nano structures on Pd(100), thin CuPd and AgPd films on inert Ru(0001), and at interfaces. The disorder broadening on CLS due to local environment effects was calculated in selected alloys.A part of the thesis concern investigations related to the magnetic ordering in Invar alloys, including the influence of local environment effects. A study was made for the dependence of effective exchange parameter on the electron concentration, volume and local chemical composition.
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| 20. |
- Olovsson, Weine, et al.
(författare)
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Interface core-level shifts as a probe of embedded thin-film quality
- 2011
-
Ingår i: Physical Review B. Condensed Matter and Materials Physics. - : American Physical Society. - 1098-0121 .- 1550-235X. ; 84:8, s. 085431-
-
Tidskriftsartikel (refereegranskat)abstract
- We use first-principles calculations of layer-resolved core-level binding energy shifts (CLSs) within density functional theory as away to characterize the interface quality and thickness in embedded thin-film nanomaterials. A closer study of interfaces is motivated as properties specific to nanostructures can be related directly to the interface environment or indirectly as interference effects due to quantum confinement. From an analysis based on the Cu 2p(3/2) CLS for Cu embedded in Ni and Co fcc (100) and Fe bcc (100), with the interfaces represented by intermixing profiles controlled by a single parameter, we evaluate layer-resolved shifts as a probe of the thin-film quality. The core-level shifts in the corresponding disordered alloys, as well as local environment effects, are studied for comparison. We also discuss the possibility of detecting interface states by means of core-level shift measurements.
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| 21. |
- Olovsson, Weine, et al.
(författare)
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Rhombohedral and Turbostratic Boron Nitride Polytypes Investigated by X-ray Absorption Spectroscopy
- 2022
-
Ingår i: The Journal of Physical Chemistry C. - : AMER CHEMICAL SOC. - 1932-7447 .- 1932-7455. ; 126, s. 21101-21108
-
Tidskriftsartikel (refereegranskat)abstract
- The electronic structure of rhombohedral sp2-hybridized boron nitride (r-BN) is characterized by X-ray absorption near-edge structure spectroscopy. Measurements are performed at the boron and nitrogen K-edges (1s) and interpreted with first-principles density functional theory calculations, including final state effects by applying a core hole. We show that it is possible to distinguish between different 2D planar polytypes such as rhombohedral, twinned rhombohedral, hexagonal, and turbostratic BN by the difference in chemical shifts. In particular, the chemical shift at the B 1s-edge is shown to be significant for the turbostratic polytype. This implies that the band gap can be tuned by a superposition of different polytypes and stacking of lattice planes.
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| 22. |
- Olovsson, Weine, et al.
(författare)
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Structure and Bonding in Amorphous Cr1−xCx Nanocomposite Thin Films: X‐ray Absorption Spectra and First-Principles Calculations
- 2016
-
Ingår i: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 120:23, s. 12890-12899
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Tidskriftsartikel (refereegranskat)abstract
- The local structure and chemical bonding in two-phase amorphous Cr1−xCx nanocomposite thin films are investigated by Cr K-edge (1s) X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) spectroscopies in comparison to theory. By utilizing the computationally efficient stochastic quenching (SQ) technique, we reveal the complexity of different Cr-sites in the transition metal carbides, highlighting the need for large scale averaging to obtain theoretical XANES and EXAFS spectra for comparison with measurements. As shown in this work, it is advantageous to use ab initio theory as an assessment to correctly model and fit experimental spectra and investigate the trends of bond lengths and coordination numbers in complex amorphous materials. With sufficient total carbon content (≥30 at. %), we find that the short-range coordination in the amorphous carbide phase exhibit similarities to that of a Cr7C3 ± y structure, while excessive carbons assemble in the amorphous carbon phase.
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| 23. |
- Olovsson, Weine, et al.
(författare)
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The Be K-edge in beryllium oxide and chalcogenides : soft x-ray absorption spectra from first-principles theory and experiment
- 2013
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Ingår i: Journal of Physics. - : Institute of Physics: Hybrid Open Access. - 0953-8984 .- 1361-648X. ; 25:31
-
Tidskriftsartikel (refereegranskat)abstract
- We have carried out a theoretical and experimental investigation of the beryllium K-edge soft x-ray absorption fine structure of beryllium compounds in the oxygen group, considering BeO, BeS, BeSe, and BeTe. Theoretical spectra are obtained ab initio, through many-body perturbation theory, by solving the Bethe–Salpeter equation (BSE), and by supercell calculations using the core-hole approximation. All calculations are performed with the full-potential linearized augmented plane-wave method. It is found that the two different theoretical approaches produce a similar fine structure, in good agreement with the experimental data. Using the BSE results, we interpret the spectra, distinguishing between bound core-excitons and higher energy excitations.
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| 24. |
- Olovsson, Weine, 1975-, et al.
(författare)
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Vibrational Effects in X-ray Absorption Spectra of Two-Dimensional Layered Materials
- 2019
-
Ingår i: The Journal of Physical Chemistry C. - : ACS Publications. - 1932-7447 .- 1932-7455. ; 123:15, s. 9688-9692
-
Tidskriftsartikel (refereegranskat)abstract
- With the examples of the C K-edge in graphite and the B K-edge in hexagonal boron nitride, we demonstrate the impact of vibrational coupling and lattice distortions on the X-ray absorption near-edge structure (XANES) in two-dimensional layered materials. Theoretical XANES spectra are obtained by solving the Bethe–Salpeter equation of many-body perturbation theory, including excitonic effects through the correlated motion of the core hole and excited electron. We show that accounting for zero-point motion is important for the interpretation and understanding of the measured X-ray absorption fine structure in both materials, in particular for describing the σ*-peak structure.
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| 25. |
- Osinger, Barbara, et al.
(författare)
-
Charge transfer effects in (HfNbTiVZr)C – shown by ab-initio calculations and X-ray photoelectron spectroscopy
-
Tidskriftsartikel (övrigt vetenskapligt/konstnärligt)abstract
- Considering charge transfer effects and the variability of the bonding between elements with different electronegativity opens up a deeper understanding of the electronic structure and as a result many of the properties in high entropy related materials. This study investigates the importance of the diverse bonding and chemical environments when discussing multicomponent carbide materials. A combination of ab initio calculations and X-ray photoelectron spectroscopy (XPS) was used to investigate the electronic structure of multicomponent thin films based on the (HfNbTiVZr)C system. The charge transfer was quantified theoretically using relaxed and non-relaxed multicomponent as well as binary carbide reference structures, employing a fixed sphere model. High-resolution XPS spectra from (HfNbTiVZr)C magnetron sputtered thin films displayed core level binding energy shifts and broadening effects as a result of the complex chemical environment. Charge transfer effects and a changed electronic structure in the multicomponent material, compared with the reference binary carbides, are observed both experimentally and in the DFT simulations. The observed effects loosely follow electronegativity considerations, leading to a deviation from an ideal solid solution structure assuming non-distinguishable chemically equivalent environments.
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| 26. |
- Osinger, Barbara, et al.
(författare)
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Charge transfer effects in (HfNbTiVZr)C-Shown by ab initio calculations and X-ray photoelectron spectroscopy
- 2024
-
Ingår i: Journal of The American Ceramic Society. - : WILEY. - 0002-7820 .- 1551-2916.
-
Tidskriftsartikel (refereegranskat)abstract
- Considering charge transfer effects and the variability of the bonding between elements with different electronegativity opens up a deeper understanding of the electronic structure and as a result many of the properties in high entropy-related materials. This study investigates the importance of the diverse bonding and chemical environments when discussing multicomponent carbide materials. A combination of ab initio calculations and X-ray photoelectron spectroscopy (XPS) was used to investigate the electronic structure of multicomponent thin films based on the (HfNbTiVZr)C system. The charge transfer was quantified theoretically using relaxed and nonrelaxed multicomponent as well as binary carbide reference structures, employing a fixed sphere model. High-resolution XPS spectra from (HfNbTiVZr)C magnetron-sputtered thin films displayed core-level binding energy shifts and broadening effects as a result of the complex chemical environment. Charge transfer effects and a changed electronic structure in the multicomponent material, compared with the reference binary carbides, are observed both experimentally and in the density functional theory (DFT) simulations. The observed effects loosely follow electronegativity considerations, leading to a deviation from an ideal solid solution structure assuming nondistinguishable chemically equivalent environments.
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| 27. |
- Ritchie, Andrew, et al.
(författare)
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Strain sensitivity in the nitrogen 1s NEXAFS spectra of gallium nitride
- 2014
-
Ingår i: Applied Surface Science. - : Elsevier. - 0169-4332 .- 1873-5584. ; 316, s. 232-236
-
Tidskriftsartikel (refereegranskat)abstract
- The nitrogen 1s near edge X-ray absorption fine structure (NEXAFS) of gallium nitride (GaN) shows astrong natural linear dichroism that arises from its anisotropic wurtzite structure. An additional spectro-scopic variation arises from lattice strain in epitaxially grown GaN thin films. This variation is directlyproportional to the degree of strain for some spectroscopic features. This strain variation is interpretedwith the aid of density functional theory calculations.
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| 28. |
- Shu, Rui, 1990-, et al.
(författare)
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Stoichiometry Effects on the Chemical Ordering and Superconducting Properties in TiZrTaNbNx Refractory High Entropy Nitrides
- 2023
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Ingår i: Annalen der Physik. - : Wiley-VCH Verlagsgesellschaft. - 0003-3804 .- 1521-3889.
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Tidskriftsartikel (refereegranskat)abstract
- High-entropy materials, an exciting new class of structural materials involvingfive or more elements, are emerging as unexplored ground forsuperconductors. Here, the effects of nitrogen stoichiometry are investigatedon local chemical structure of TiZrNbTa-based thin films by variousX-ray-based techniques. Lattice distortion and short-range order of a set ofTiZrNbTaNxsamples, including bond lengths of different atomic pairs andcoordination numbers of substituting atoms are quantitatively studied. Themaximum superconducting transition temperature Tcis found at 10 K for anear-stoichiometric (TiZrNbTa)N1.08film, which is>8 K measured for ametallic TiZrNbTa film. The underlying electronic structure and chemicalbonding in these high entropy nitrides thus influence the superconductingmacroscopic properties.
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| 29. |
- Tal, Alexey, 1990-
(författare)
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Electronic and structural properties of nanoclusters
- 2018
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Nanoclusters have gained a huge interest due to their unique properties. They represent an intermediate state between an atom and a solid, which manifests itself in their atomic configurations and electronic structure. The applications of nanoclusters require detailed understanding of their properties and strongly depend on the ability to control their synthesis process. Significant effort has been invested in modelling of nanoclusters properties. However, the complexity of these systems is such that many aspects of their growth process and properties are yet to be understood.My thesis focuses on describing structural and electronic properties of nanoclusters. In particular, the model for nanoparticles growth in plasma condition is developed and applied, allowing to describe the influence of the plasma conditions on the evaporation, growth and morphological transformation processes. The mechanism driving the morphology transition from icosahedral to decahedral phase is suggested based on force-fields models. Spectroscopic methods allow for precise characterization of nanoclusters and constitute an important tool for analysis of their electronic structure of valence band as well as core-states. The special attention in the thesis is paid to the core-states of nanoclusters and influences that affect them. In particular, the effects of local coordination, interatomic distances and confinement effects are investigated in metal nanoclusters by density functional theory methods. These effects and their contribution to spectroscopic features of nanoclusters in X-ray photoemission are modelled. The relation between the reactivity of nanoclusters and their spectroscopic features calculated in different approximations are revealed and explained. Ceria is a very important system for many applications due to the ability of cerium atoms to change their oxidation state depending on the environment. The shift of the oxidation state and its effects on the core-states is examined with X-ray absorption measurements and modelling allowing to build a rigid foundation for interpretation of the measured spectra and characterization of electronic structure of ceria nanoparticles.
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| 30. |
- Tal, Alexey, et al.
(författare)
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Origin of the core-level binding energy shifts in Au nanoclusters
- 2017
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Ingår i: Physical Review B. - : AMER PHYSICAL SOC. - 2469-9950 .- 2469-9969. ; 95:24
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Tidskriftsartikel (refereegranskat)abstract
- We investigate the shifts of the core-level binding energies in small gold nanoclusters by using ab initio density-functional-theory calculations. The shift of the 4f states is calculated for magic-number nanoclusters in a wide range of sizes and morphologies. We find a nonmonotonous behavior of the core-level shift in nanoclusters depending on the size. We demonstrate that there are three main contributions to the Au 4f shifts, which depend sensitively on the interatomic distances, coordination, and quantum confinement. They are identified and explained by the change of the on-site electrostatic potential.
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| 31. |
- Tomita, Kota, et al.
(författare)
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Core-Exciton Interaction in Sodium L-2,L-3 edge Structure Investigated Using the Bethe-Salpeter Equation
- 2016
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Ingår i: The Journal of Physical Chemistry C. - : AMER CHEMICAL SOC. - 1932-7447 .- 1932-7455. ; 120:17, s. 9036-9042
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Tidskriftsartikel (refereegranskat)abstract
- Despite the importance of sodium compounds for their application in sodium-ion rechargeable batteries, core-exciton interactions in sodium L-2,L-3 edge core-electron loss spectra are not well-understood. In this study, Bethe-Salpeter equation calculations of sodium L-2,L-3 edges of sodium compounds were performed to understand the relationships between the core-exciton interactions and the electronic structure of sodium compounds. It was revealed that the core-exciton interaction of sodium compounds is strongly dependent on the compounds. We found that neither band gap nor ionic charge can explain the trend; however, the transition energy shows a clear correlation to the magnitude of the core-exciton interaction. These results indicate that the magnitude of the core-exciton interaction is decided by the excited electronic structure of each compound.
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| 32. |
- Tomita, Kota, et al.
(författare)
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Strong excitonic interactions in the oxygen K-edge of perovskite oxides
- 2017
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Ingår i: Ultramicroscopy. - : ELSEVIER SCIENCE BV. - 0304-3991 .- 1879-2723. ; 178, s. 105-111
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Tidskriftsartikel (refereegranskat)abstract
- Excitonic interactions of the oxygen IC edge electron energy-loss near-edge structure (ELNES) of perovskite oxides, CaTiO3, SrTiO3, and BaTiO3, together with reference oxides, MgO, CaO, SrO, BaO, and TiO2, were investigated using a first -principles Bethe-Salpeter equation calculation. Although the transition energy of oxygen K-edge is high, strong excitonic interactions were present in the oxygen K-edge ELNES of the perovskite oxides, whereas the excitonic interactions were negligible in the oxygen IC edge ELNES of the reference compounds. Detailed investigation of the electronic structure suggests that the strong excitonic interaction in the oxygen K-edge ELNES of the perovskite oxides is caused by the directionally confined, low-dimensional electronic structure at the Ti-O-Ti bonds. (C) 2016 Elsevier B.V. All rights reserved.
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| 33. |
- Wang, Weimin, et al.
(författare)
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Band structure of hydrogenated silicene on Ag(111): Evidence for half-silicane
- 2016
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Ingår i: PHYSICAL REVIEW B. - : AMER PHYSICAL SOC. - 2469-9950. ; 93:8, s. 081406-
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Tidskriftsartikel (refereegranskat)abstract
- In the case of graphene, hydrogenation removes the conductivity due to the bands forming the Dirac cone by opening up a band gap. This type of chemical functionalization is of the utmost importance for electronic applications. As predicted by theoretical studies, a similar change in the band structure is expected for silicene, the closest analog to graphene. We here report a study of the atomic and electronic structures of hydrogenated silicene with hydrogen on one side, the so-called half-silicane. The ("2 root 3 x 2 root 3") phase of silicene on Ag(111) was used in this Rapid Communication since it can be formed homogeneously across the entire surface of the Ag substrate. Low-energy electron diffraction and scanning tunneling microscopy data clearly show that hydrogenation changes the structure of silicene on Ag(111) resulting in a (1 x 1) periodicity with respect to the silicene lattice. The hydrogenated silicene also exhibits a quasiregular ("2 root 3 x 2 root 3")-like arrangement of vacancies. Angle-resolved photoelectron spectroscopy revealed two dispersive bands which can be unambiguously assigned to half-silicane. The common top of these bands is located at similar to 0.9 eV below the Fermi level. We find that the experimental bands are closely reproduced by the theoretical band structure of free-standing silicene with H adsorbed on the upper hexagonal sublattice.
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| 34. |
- Wang, Weimin, et al.
(författare)
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Experimental and theoretical determination of sigma bands on ("2 root 3 x 2 root 3") silicene grown on Ag(111)
- 2015
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Ingår i: Physical Review B. Condensed Matter and Materials Physics. - : AMER PHYSICAL SOC. - 1098-0121 .- 1550-235X. ; 92:20, s. 205427-
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Tidskriftsartikel (refereegranskat)abstract
- Silicene, the two-dimensional (2D) allotrope of silicon, has very recently attracted a lot of attention. It has a structure that is similar to graphene and it is theoretically predicted to show the same kind of electronic properties which have put graphene into the focus of large research and development projects worldwide. In particular, a 2D structure made from Si is of high interest because of the application potential in Si-based electronic devices. However, so far there is not much known about the silicene band structure from experimental studies. A comprehensive study is here presented of the atomic and electronic structure of the silicene phase on Ag(111) denoted as (2 root 3 x 2 root 3)R30 degrees in the literature. Low energy electron diffraction (LEED) shows an unconventional rotated ("2 root 3 x 2 root 3") pattern with a complicated set of split diffraction spots. Scanning tunneling microscopy (STM) results reveal a Ag(111) surface that is homogeneously covered by the ("2 root 3 x 2 root 3") silicene which exhibits an additional quasiperiodic long-range ordered superstructure. The complex structure, revealed by STM, has been investigated in detail and we present a consistent picture of the silicene structure based on both STM and LEED. The homogeneous coverage by the ("2 root 3 x 2 root 3") silicene facilitated an angle-resolved photoelectron spectroscopy study which reveals a silicene band structure of unprecedented detail. Here we report four silicene bands which are compared to calculated dispersions based on a relaxed (2 root 3 x 2 root 3) model. We find good qualitative agreement between the experimentally observed bands and calculated silicene bands of sigma character.
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| 35. |
- Xia, Chao, 1986-, et al.
(författare)
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Effects of rhenium on graphene grown on SiC(0001)
- 2018
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Ingår i: Journal of Electron Spectroscopy and Related Phenomena. - : Elsevier. - 0368-2048 .- 1873-2526. ; 222, s. 117-121
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Tidskriftsartikel (refereegranskat)abstract
- We study the effects of Rhenium (Re) deposited on epitaxial monolayer graphene grown on SiC(0001) and after subsequent annealing at different temperatures, by performing high resolution photoelectron spectroscopy (PES) and angle resolved photoelectron spectroscopy (ARPES). The graphene-Re system is found to be thermally stable. While no intercalation or chemical reaction of the Re is detected after deposition and subsequent annealing up to 1200 degrees C, a gradual decrease in the binding energy of the Re 4f doublet is observed. We propose that a larger mobility of the Re atoms with increasing annealing temperature and hopping of Re atoms between different defective sites on the graphene sample could induce this decrease of Re 4f binding energy. This is corroborated by first principles density functional theory (DFT) calculations of the Re core-level binding energy shift. No change in the doping or splitting of the initial monolayer graphene electronic band structure is observed after Re deposition and annealing up to 1200 degrees C, only a broadening of the bands. (C) 2017 Elsevier B.V. All rights reserved.
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