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Alfred Q. R. Baron

Publications and source records attributed to Alfred Q. R. Baron.

33 records · Page 2Linked to original sources

Spin-orbit coupling effects on spin-phonon coupling in Cd2Os2O7

Spin-orbit coupling (SOC) is essential in understanding the properties of 5d transition metal compounds, whose SOC value is large and almost comparable to other key parameters. Over the past few years, there have been numerous studies on the SOC-driven effects of the electronic bands, magnetism, and spin-orbit entanglement for those materials with a large SOC. However, it is less studied and remains an unsolved problem in how the SOC affects the lattice dynamics. We, therefore, measured the phonon spectra of 5d pyrochlore Cd2Os2O7 over the full Brillouin zone to address the question by using inelastic x-ray scattering (IXS). Our main finding is a visible mode-dependence in the phonon spectra, measured across the metal-insulator transition at 227 K. We examined the SOC strength dependence of the lattice dynamics and its spin-phonon (SP) coupling, with first-principle calculations. Our experimental data taken at 100 K are in good agreement with the theoretical results obtained with the optimized U = 2.0 eV with SOC. By scaling the SOC strength and the U value in the DFT calculations, we demonstrate that SOC is more relevant than U to explaining the observed mode-dependent phonon energy shifts with temperature. Furthermore, the temperature dependence of the phonon energy can be effectively described by scaling SOC. Our work provides clear evidence of SOC producing a non-negligible and essential effect on the lattice dynamics of Cd2Os2O7 and its SP coupling.

cond-mat.mtrl-sci↗

Introduction to High-Resolution Inelastic X-Ray Scattering

This paper reviews non-resonant, meV-resolution inelastic x-ray scattering (IXS), as applied to the measurement of atomic dynamics of crystalline materials. It is designed to be an introductory, though in-depth, look at the field for those who be may interested in performing IXS experiments, or in understanding the operation of IXS spectrometers, or those desiring a practical introduction to harmonic phonons in crystals at finite momentum transfers. The treatment of most topics begins from ground-level, with a strong emphasis on practical issues, as they have occurred to the author in two decades spent introducing meV-resolved IXS in Japan, including designing and helping to build two IXS beamlines, spectrometers and associated instrumentation, performing experiments, and helping and teaching other scientists. After an introduction that compares IXS to other methods of investigating atomic dynamics, some of the basic principles of scattering theory are described with the aim of introducing useful and relevant concepts for the experimentalist. That section includes a fairly detailed discussion of harmonic phonons. The theory section is followed by a brief discussion of calculations and then a longer section on spectrometer design, concepts, and implementation, including a brief introduction to dynamical diffraction and a survey of presently available instruments. Finally, there is discussion of the types of experiments that have been carried out, with a focused discussion on measurements of superconductors, and brief discussion (but with many references) of other types of crystalline samples.

cond-mat.mtrl-sci↗

Nonlinear resonant X-ray Raman scattering

We report the observation of a novel nonlinear effect in the hard x-ray range. Upon illuminating Fe and Cu metal foils with intense x-ray pulses tuned near their respective K edges, photons at nearly twice the incoming photon energy are emitted. The signal rises quadratically with the incoming intensity, consistent with two-photon excitation. The spectrum of emitted high-energy photons comprises multiple Raman lines that disperse with the incident photon energy. Upon reaching the double K-shell ionization threshold, the signal strength undergoes a marked rise. Above this threshold, the lines cease dispersing, turning into orescence lines with energies much greater than obtainable by single electron transitions, and additional Raman lines appear. We attribute these processes to electron-correlation mediated multielectron transitions involving double-core hole excitation and various two-electron de-excitation processes to a final state involving one or more L and M core-holes.

physics.atom-ph↗

Furnace for Inelastic X-Ray Scattering from Liquids to 1600C

The design and implementation of a furnace for inelastic x-ray scattering from liquids with sample temperatures up to ~1600C is described. Carbon composite heaters operating in vacuum provide robust heating elements: one pair of heaters has been used for >18 days of operational time above 1500C, including 8 cycles to room temperature. High quality data has been obtained to scattering angles as low as 7 mrad in two-theta (Q<1 nm-1 at 25.7 keV) from a sample at 1560C.

physics.ins-det↗

Lattice dynamics in FeSe via inelastic x-ray scattering and first-principles calculations

We report an inelastic x-ray scattering investigation of phonons in FeSe superconductor. Comparing the experimental phonon dispersion with density functional theory (DFT) calculations in the non-magnetic state, we found a significant disagreement between them. Improved overall agreement was obtained by allowing for spin-polarization in the DFT calculations, despite the absence of magnetic order in the experiment. This calculation gives a realistic approximation, at DFT level, of the disordered paramagnetic state of FeSe, in which strong spin fluctuations are present.

cond-mat.supr-con↗

Auxiliary Optics For meV-IXS at SPring-8: KB, Analyzer Masks, Soller Slit & Screen, BPM

This paper discusses several optical elements now in use at BL43LXU, the RIKEN Quantum NanoDynamics Beamline, of the RIKEN SPring-8 Center. BL43LXU is dedicated to meV-resolved inelastic x-rays scattering using spherical analyzers operating between 15.8 and 25.7 keV. The work described here is relevant for setups on the high-resolution spectrometer (10m two-theta arm) with resolution between 2.8 and 0.8 meV. Specific optics discussed include a multilayer Kirkpatrick-Baez (KB) mirror pair that focuses the full (~1x3mm2) beam at 17.79 keV to a 4.4 X 4.1 μm2 spot with ~60% throughput, two different types of Soller slits that help reduce backgrounds, masks for the analyzers that allow increased solid angle to be collected while preserving momentum resolution, and a diamond quadrant beam position monitor (BPM). These elements have been used and facilitate experiments in extreme conditions with diamond anvil cells, and liquid measurements at low momentum transfers, among other work.

physics.ins-det↗

Phonon anomalies with doping in superconducting oxychlorides Ca2-xCuO2Cl2

We measure the dispersion of the Cu-O bond-stretching phonon mode in the high-temperature superconducting parent compound Ca$_2$CuO$_2$Cl$_2$. Our density functional theory calculations predict a cosine-shaped bending of the dispersion along both the ($ξ$00) and ($ξξ$0) directions, while comparison with previous results on Ca$_{1.84}$CuO$_2$Cl$_2$ show it only along ($ξ$00), suggesting an anisotropic effect which is not reproduced in calculation at optimal doping. Comparison with isostructural La$_{2-x}$Sr$_x$CuO$_4$ suggests that these calculations reproduce well the overdoped regime, however they overestimate the doping effect on the Cu-O bond-stretching mode at optimal doping.

cond-mat.str-el↗

Scientific Opportunities with an X-ray Free-Electron Laser Oscillator

An X-ray free-electron laser oscillator (XFELO) is a new type of hard X-ray source that would produce fully coherent pulses with meV bandwidth and stable intensity. The XFELO complements existing sources based on self-amplified spontaneous emission (SASE) from high-gain X-ray free-electron lasers (XFEL) that produce ultra-short pulses with broad-band chaotic spectra. This report is based on discussions of scientific opportunities enabled by an XFELO during a workshop held at SLAC on June 29 - July 1, 2016

physics.ins-det↗

Lattice and Magnetic Effects on a d-d Excitation in NiO Using a 25 meV Resolution X-ray Spectrometer

We investigate the behavior of a $d$-$d$ transition in NiO using a new x-ray spectrometer with 0.025 eV resolution at 15816 eV, and via ab-initio ligand field theory calculations. The transition at ~1.7 eV energy transfer is measured at temperatures between 20 and 800 K, at a momentum transfer |$\bf{Q}$| = 6.52 Å$^{-1}$. Fine structure is clearly observed at 20 K. As temperature is increased, the excitation shifts to lower energy and broadens. We explain the energy shift as being related to thermal expansion and to magnetism. The broadening is well fit considering thermal fluctuations of the Ni-O bond length, with a scale factor found to be in reasonable agreement with calculation.

cond-mat.str-el↗

Signature of a polyamorphic transition in the THz spectrum of vitreous GeO2

The THz spectrum of density fluctuations, $S(Q, ω)$, of vitreous GeO$_2$ at ambient temperature was measured by inelastic x-ray scattering from ambient pressure up to pressures well beyond that of the known $α$-quartz to rutile polyamorphic (PA) transition. We observe significant differences in the spectral shape measured below and above the PA transition, in particular, in the 30-80 meV range. Guided by first-principle lattice dynamics calculations, we interpret the changes in the phonon dispersion as the evolution from a quartz-like to a rutile-like coordination. Notably, such a crossover is accompanied by a cusp-like behavior in the pressure dependence of the elastic response of the system. Overall, the presented results highlight the complex fingerprint of PA phenomena on the high-frequency phonon dispersion.

cond-mat.dis-nn↗

Non-complicated EuTiO3 Structure

A recently published paper [arXiv:1206.5417 ]showed strong incommensurate diffraction peaks in EuTiO3 around zone boundary R-points. We wish to convey that in our samples, and, it seems, at least another case from the literature, these peaks are absent.

cond-mat.str-el↗

Phonon Softening and Dispersion in EuTiO3

We measured phonon dispersion in single crystal EuTiO$_3$ using inelastic x-ray scattering. A structural transition to an antiferrodistortive phase was found at a critical temperature $T_0$=287$\pm$1 K using powder and single-crystal x-ray diffraction. Clear softening of the zone boundary \emph{R}-point \textbf{q}=(0.5 0.5 0.5) acoustic phonon shows this to be a displacive transition. The mode energy plotted against reduced temperature could be seen to nearly overlap that of $\rm SrTiO_3$, suggesting a universal scaling relation. Phonon dispersion was measured along $Γ$-$X$ (0 0 0)$\rightarrow$(0.5 0 0). Mode eigenvectors were obtained from a shell model consistent with the \textbf{q}-dependence of intensity and energy, which also showed that the dispersion is nominally the same as in $\rm SrTiO_3$ at room temperature, but corrected for mass. The lowest energy optical mode, determined to be of Slater character, softens approximately linearly with temperature until the 70-100 K range where the softening stops, and at low temperature, the mode disperses linearly near the zone center.

cond-mat.str-el↗

Effect of K Doping on Phonons in Ba1-xKxFe2As2

The lattice dynamics of Ba1-xKxFe2As2 (x = 0.00, 0.27) have been studied by inelastic X-ray scattering measurement at room temperature. K doping induces the softening and broadening of phonon modes in the energy range E = 10-15 meV. Analysis with a Born-von Karman force-constant model indicates that the softening results from reduced interatomic force constants around (Ba,K) sites following the displacement of divalent Ba by monovalent K. The phonon broadening may be explained by the local distortions induced by the K substitution. Extra phonon modes are observed around the wave vector q = (0.5,0,0) at E = 16.5 meV for the x = 0.27 sample. These modes may arise either from the local disorder induced by K doping or from electron-phonon coupling.

cond-mat.supr-con↗

Phonons in Crystals using Inelastic X-Ray Scattering

The use of inelastic x-ray scattering (IXS) to investigate phonons and phonon dispersion in crystals opens the field of phonon spectroscopy, allowing measurements on tiny samples: micrograms of material, or single crystals ~10 to 100 micron diameter are sufficient. Here we review the technique as it is practiced at BL35XU of SPring-8, in Hyogo prefecture. An introduction is provided that is aimed at potential IXS users, highlighting the unique and advantageous aspects of the technique. Present work, including several example experiments, and future directions are discussed.

cond-mat.mtrl-sci↗