Layer dependent band dispersion and correlations using tunable Soft X-ray ARPES

Soft X-ray Angle-Resolved Photoemission Spectroscopy is applied to study in-plane band dispersions of Nickel as a function of probing depth. Photon energies between 190 and 780 eV were used to effectively probe up to 3-7 layers. The results show layer dependent band dispersion of the Delta_2 minority-spin band which crosses the Fermi level in 3 or more layers, in contrast to known top 1-2 layers dispersion obtained using ultra-violet rays. The layer dependence corresponds to an increased value of exchange splitting and suggests reduced correlation effects in the bulk compared to the surface.Comment: 7 pages, 3 figures Revised text and figur

Direct Observation of Site-specific Valence Electronic Structure at Interface: SiO2/Si Interface

Atom specific valence electronic structures at interface are elucidated successfully using soft x-ray absorption and emission spectroscopy. In order to demonstrate the versatility of this method, we investigated SiO2/Si interface as a prototype and directly observed valence electronic states projected at the particular atoms of the SiO2/Si interface; local electronic structure strongly depends on the chemical states of each atom. In addition we compared the experimental results with first-principle calculations, which quantitatively revealed the interfacial properties in atomic-scale.Comment: 4 pages, 3 figure

Doping Dependent Changes in Nitrogen 2pp States in the Diluted Magnetic Semiconductor Ga1−x_{1-x}Crx_{x}N

We study the electronic structure of the recently discovered diluted magnetic semiconductor Ga$_{1-x}$Cr$_{x}$N ($x$ = 0.01-0.10). A systematic study of the changes in the $occupied$ and $unoccupied$ ligand (N) partial density of states (DOS) of the host lattice is carried out using N 1$s$ soft x-ray emission and absorption spectroscopy, respectively. X-ray absorption measurements confirm the wurtzite N 2$p$ DOS and substitutional doping of Cr into Ga-sites. Coupled changes in the $occupied$ and $unoccupied$ N 2$p$ character DOS of Ga$_{1-x}$Cr$_{x}$N identify states responsible for ferromagnetism consistent with band structure calculations.Comment: 5 pages, 4 figures, submitted to Phys. Rev.

Immittance Matching for Multi-dimensional Open-system Photonic Crystals

An electromagnetic (EM) Bloch wave propagating in a photonic crystal (PC) is characterized by the immittance (impedance and admittance) of the wave. The immittance is used to investigate transmission and reflection at a surface or an interface of the PC. In particular, the general properties of immittance are useful for clarifying the wave propagation characteristics. We give a general proof that the immittance of EM Bloch waves on a plane in infinite one- and two-dimensional (2D) PCs is real when the plane is a reflection plane of the PC and the Bloch wavevector is perpendicular to the plane. We also show that the pure-real feature of immittance on a reflection plane for an infinite three-dimensional PC is good approximation based on the numerical calculations. The analytical proof indicates that the method used for immittance matching is extremely simplified since only the real part of the immittance function is needed for analysis without numerical verification. As an application of the proof, we describe a method based on immittance matching for qualitatively evaluating the reflection at the surface of a semi-infinite 2D PC, at the interface between a semi-infinite slab waveguide (WG) and a semi-infinite 2D PC line-defect WG, and at the interface between a semi-infinite channel WG and a semi-infinite 2D PC slab line-defect WG.Comment: 8 pages, 6 figure

Probing the Hofmeister Effect with Ultrafast Core Hole Spectroscopy

In the current work, X-ray emission spectra of aqueous solutions of different inorganic salts within the Hofmeister series are presented. The results reflect the direct interaction of the ions with the water molecules and therefore, reveal general properties of the salt-water interactions. Within the experimental precision a significant effect of the ions on the water structure has been observed but no ordering according to the structure maker/structure breaker concept could be mirrored in the results indicating that the Hofmeister effect-if existent-may be caused by more complex interactions

X ray emission spectroscopy of bulk liquid water in no man s land

The structure of bulk liquid water was recently probed by x ray scattering below the temperature limit of homogeneous nucleation TH of amp; 8764;232 K [J. A. Sellberg et al., Nature 510, 381 384 2014 ]. Here, we utilize a similar approach to study the structure of bulk liquid water below TH using oxygen K edge x ray emission spectroscopy XES . Based on previous XES experiments [T. Tokushima et al., Chem. Phys. Lett. 460, 387 400 2008 ] at higher temperatures, we expected the ratio of the 1b1 amp; 8242; and 1b1 amp; 8242; amp; 8242; peaks associated with the lone pair orbital in water to change strongly upon deep supercooling as the coordination of the hydrogen H bonds becomes tetrahedral. In contrast, we observed only minor changes in the lone pair spectral region, challenging an interpretation in terms of two interconverting species. A number of alternative hypotheses to explain the results are put forward and discussed. Although the spectra can be explained by various contributions from these hypotheses, we here emphasize the interpretation that the line shape of each component changes dramatically when approaching lower temperatures, where, in particular, the peak assigned to the proposed disordered component would become more symmetrical as vibrational interference becomes more importan

Nanoscale Dynamics of Phase Flipping in Water near its Hypothesized Liquid-Liquid Critical Point

Achieving a coherent understanding of the many thermodynamic and dynamic anomalies of water is among the most important unsolved puzzles in physics, chemistry, and biology. One hypothesized explanation imagines the existence of a line of first order phase transitions separating two liquid phases and terminating at a novel "liquid-liquid" critical point in a region of low temperature ($T \approx 250 \rm{K}$) and high pressure ($P \approx 200 \rm{MPa}$). Here we analyze a common model of water, the ST2 model, and find that the entire system flips between liquid states of high and low density. Further, we find that in the critical region crystallites melt on a time scale of nanoseconds. We perform a finite-size scaling analysis that accurately locates both the liquid-liquid coexistence line and its associated liquid-liquid critical point.Comment: 22 pages, 5 figure

Ab initio van der Waals interactions in simulations of water alter structure from mainly tetrahedral to high-density-like

The structure of liquid water at ambient conditions is studied in ab initio molecular dynamics simulations using van der Waals (vdW) density-functional theory, i.e. using the new exchange-correlation functionals optPBE-vdW and vdW-DF2. Inclusion of the more isotropic vdW interactions counteracts highly directional hydrogen-bonds, which are enhanced by standard functionals. This brings about a softening of the microscopic structure of water, as seen from the broadening of angular distribution functions and, in particular, from the much lower and broader first peak in the oxygen-oxygen pair-correlation function (PCF), indicating loss of structure in the outer solvation shells. In combination with softer non-local correlation terms, as in the new parameterization of vdW-DF, inclusion of vdW interactions is shown to shift the balance of resulting structures from open tetrahedral to more close-packed. The resulting O-O PCF shows some resemblance with experiment for high-density water (A. K. Soper and M. A. Ricci, Phys. Rev. Lett., 84:2881, 2000), but not directly with experiment for ambient water. However, an O-O PCF consisting of a linear combination of 70% from vdW-DF2 and 30% from experiment on low-density liquid water reproduces near-quantitatively the experimental O-O PCF for ambient water, indicating consistency with a two-liquid model with fluctuations between high- and low-density regions