Search

In this work, we investigate the possibility of controlling the acoustic damping in a liquid when nanoparticles are suspended in it. To shed light on this topic, we performed Inelastic X-Ray Scattering (IXS) measurements of the terahertz collective dynamics of aqueous suspensions of nanospheres of various materials, size, and relative concentration, either charged or neutral. A Bayesian analysis of measured spectra indicates that the damping of the two acoustic modes of water increases upon nanoparticle immersion. This effect seems particularly pronounced for the longitudinal acoustic mode, which, whenever visible at all, rapidly damps off when increasing the exchanged wavevector. Results also indicate that the observed effect strongly depends on the material the immersed nanoparticles are made of.

Significance Unveiling the unusual atomic dynamics in superionic conductors is critical for the design of energy conversion and storage materials, for example to rationalize their thermal transport properties in thermoelectric applications or their fast ionic conductivity in solid-state electrolytes. We combine neutron/X-ray scattering techniques with first-principles calculations to discover hybrid lattice dynamics in A g C r S e 2 , where the phonon wavelength controls the breakdown of transverse acoustic modes in the superionic phase. We attribute the ultralow thermal conductivity to strong phonon anharmonicity combined with disorder in the Ag sublattice. This understanding provides insights into the thermal conduction mechanism in superionic conductors and sheds light on the role of lattice dynamics in the emergence of superionic behavior.

Interactions between nematic fluctuations, magnetic order and superconductivity are central to the physics of iron-based superconductors. Here we report on in-plane transverse acoustic phonons in hole-doped ${\mathrm{Sr}}_{1\ensuremath{-}x}{\mathrm{Na}}_{x}{\mathrm{Fe}}_{2}{\mathrm{As}}_{2}$ measured via inelastic x-ray scattering, and extract both the nematic susceptibility and the nematic correlation length. By a self-contained method of analysis, for the underdoped ($x=0.36$) sample, which harbors a magnetically ordered tetragonal phase, we find it hosts a short nematic correlation length $\ensuremath{\xi}\ensuremath{\sim}10\text{ }\text{ }\AA{}$ and a large nematic susceptibility ${\ensuremath{\chi}}_{\mathrm{nem}}$. The optimal-doped ($x=0.55$) sample exhibits weaker phonon softening effects, indicative of both reduced $\ensuremath{\xi}$ and ${\ensuremath{\chi}}_{\mathrm{nem}}$. Our results suggest short-range nematic fluctuations may favor superconductivity, placing emphasis on the nematic correlation length for understanding the iron-based superconductors.

We used Inelastic X-ray Scattering to gain insight into the complex Terahertz dynamics of a diluted Au-nanoparticles suspension in glycerol. We observe that, albeit sparse, Au-nanoparticles leave clear signatures on the dynamic response of the system, the main one being an additional mode propagating at the nanoparticle-glycerol interface. A Bayesian inferential analysis of the lineshape reveals that such a mode, at variance with conventional acoustic modes, keeps a hydrodynamic-like behavior well beyond the continuous limit and down to sub-nanometer distances.

International audience; We used the high-resolution Inelastic X-ray Scattering beamline of the Advanced Photon Source at Argonne National Laboratory to measure the terahertz spectrum of pure water and a dilute aqueous suspension of 15 nm diameter spherical Au nanoparticles (Au-NPs). We observe that, despite their sparse volume concentration of about 0.5%, the immersed NPs strongly influence the collective molecular dynamics of the hosting liquid. We investigate this effect through a Bayesian inference analysis of the spectral lineshape, which elucidates how terahertz transport properties of water change upon Au-NP immersion. In particular, we observe a nearly complete disappearance of the longitudinal acoustic mode and a mildly decreased ability to support shear wave propagation.

The control of phonon propagation in nanoparticle arrays is one of the new frontiers of nanotechnology, potentially enabling the discovery of materials with unknown functionalities for potential innovative applications. The exploration of the terahertz window appears quite promising as phonons in this range are the leading carriers of heat transport in insulators and their control is the key to implement devices for heat flow management. Unfortunately, this scientific field is still in its infancy and even a basic topic such as the influence of floating nanoparticles on the terahertz phonon propagation of a colloidal suspension still eludes a firm answer. Shedding some light on this topic is the main motivation of the present work, which focuses an Inelastic X-Ray Scattering (IXS) measurements on a dilute suspension of Au nano-spheres in water. Measured spectra showed a non-trivial and unexpected shape displaying multiple inelastic features that, based on a Bayesian inference analysis, we assign to phonon modes propagating throughout the nanoparticle interior. Surprisingly, the spectra bear no evidence of propagating modes, which are known to dominate the spectrum of pure water, owing to the scattering that these modes suffer from the sparse nanoparticles in suspension. In perspective, this finding may inspire simple routes to manipulate high-frequency acoustic propagation in hybrid - liquid and solid- materials.

We report an experimental investigation of Yb filler ion dynamics in partially filled skutterudite samples Yb xCo 4Sb 12 ( x=0.26 and x=0.4). From extended x-ray absorption fine structure (EXAFS) measurements at the Yb L2-edge, the mean-square displacements of the Yb fillers were extracted over a wide temperature range from 10 to 500 K. We found that the low-temperature dynamics of Yb fillers are described well using a harmonic oscillator approximation with Einstein temperatures of 70±5 K for both samples. This finding is consistent with the observed low-energy phonon mode at 5.3(5) meV in the inelastic x-ray scattering (IXS) data. However, the temperature dependence deviates from the harmonic approximation at high temperatures due to significant cubic anharmonicity, which was revealed in the EXAFS cumulant analysis. Our study also demonstrates that complementary information on filler dynamics in skutterudites can be acquired using EXAFS and IXS.

The design and capabilities of the momentum-resolved high-energy-resolution inelastic X-ray spectrometer (HERIX) at beamline 30-ID of the Advanced Photon Source are reported., Inelastic X-ray scattering is a powerful and versatile technique for studying lattice dynamics in materials of scientific and technological importance. In this article, the design and capabilities of the momentum-resolved high-energy-resolution inelastic X-ray spectrometer (HERIX) at beamline 30-ID of the Advanced Photon Source are reported. The instrument operates at 23.724 keV and has an energy resolution of 1.3–1.7 meV. It can accommodate momentum transfers of up to 72 nm−1, at a typical X-ray flux of 4.5 × 109 photons s−1 meV−1 at the sample. A suite of in situ sample environments are provided, including high pressure, static magnetic fields and uniaxial strains, all at high or cryogenic temperatures.

We consider here the possibility of shaping the high-frequency acoustic propagation in a liquid upon directional confinement. This hypothesis is investigated by Inelastic X-ray Scattering measurements on water confined in aligned multi-walled carbon nanotubes, in which the momentum transfer was either parallel or orthogonal to the confinement axis. The comparison between the spectra measured in these two scattering geometries highlights the anisotropic nature of the dynamic response of directionally confined water, thus potentially inspiring new pathways to shape high-frequency sound propagation in isotropic systems. Finally, a Bayesian analysis of measured spectra unravels close similarities in the phonon dispersions of multiwalled nanotubes and graphite.

The structure and lattice dynamics of the hybrid improper ferroelectric compound ${\mathrm{Ca}}_{3\ensuremath{-}x}{\mathrm{Sr}}_{x}{\mathrm{Ti}}_{2}{\mathrm{O}}_{7}$ (for $x=0,0.6,$ and 0.9) have been studied with a combination of diffraction, inelastic scattering experiments, Raman spectroscopy, and calorimetry measurements, as well as first-principles simulations. Using inelastic neutron scattering, we have measured the phonon density of states (DOS) for $x=0.9$, which revealed a strong broadening but little change in phonon energies on heating from 10 K to 728 K across the ferroelectric phase transition temperature, ${T}_{FE}$. Using inelastic x-ray scattering, the momentum-resolved phonon dispersions were measured from 80 K to 950 K on a single crystal (for $x=0.6$), and also revealed a strong phonon broadening but a small energy shift for acoustic modes on heating across ${T}_{FE}$. Our Raman measurements (for $x=0.6$) showed robust rotational and oxygen breathing modes but soft tilt modes, consistent with previous measurements on similar compounds. Our density functional calculations achieve good agreement with both the phonon DOS and dispersions measured. We did not observe any unusual quadratic dispersion for $c$-polarized transverse acoustic modes, at odds with a recently predicted quasi-2D character, for either undoped ($x=0$) or doped ($x=0.6$) compounds.

In this Letter, we show the phonon dispersion of (CH_{3}NH_{3})_{3}Bi_{2}I_{9} single crystals at 300 K measured by inelastic x-ray scattering. The frequencies of acoustic phonons are among the lowest of crystals. Nanoindentation measurements verified that these crystals are very compliant and considerably soft. The frequency overlap between acoustic and optical phonons results in strong acoustic-optical scattering. All these features lead to an ultralow thermal conductivity. The fundamental knowledge obtained from this study will accelerate the design of novel hybrid materials for energy applications.

The Kohn anomaly and topological change of the Fermi surface in $d$-block metals can occur under high pressure with affiliated significant changes in elastic, mechanical, and transport properties. However, our understanding of their origin and associated physical phenomena remains limited both experimentally and theoretically. Here we study the pressure effect on the Kohn anomaly, electronic topological transition (ETT), and the associated anomalies in physical properties of body-centered cubic (bcc) single-crystal tantalum (Ta). The phonon dispersions of Ta crystal were directly measured up to $\ensuremath{\sim}47$ GPa using high-energy resolution inelastic x-ray scattering in a diamond anvil cell with hydrostatic helium medium. A Kohn anomaly in Ta was observed and became significantly stronger at 47.0 GPa at the reduced wave vector of $\ensuremath{\sim}0.7$ in the longitudinal acoustic mode along the [\ensuremath{\xi},0,0] direction. Our theoretical and experimental results indicate that the electron-phonon coupling and Fermi surface nesting mainly contribute to the Kohn anomaly, and the latter plays a dominant role at high pressures of 17--47 GPa. First-principles calculations further reveal an ETT with a topology change of the Fermi surface to occur at $\ensuremath{\sim}100$ GPa in Ta, which causes a softening in the elastic constants (${C}_{11}$ and ${C}_{44}$) and mechanical properties (shear, Young's, and bulk moduli). Our study shows that the $d$-orbital electrons in Ta play a key role in the stability of its electronic topological structure, where electron doping in Ta could significantly depress its ETT and elastic anomaly at high pressures. It is conceivable that our observed Kohn anomaly and ETT in a representative bcc Ta are much more prevalent in $d$-block transition metals under compression than previously thought.

Lead chalcogenides have exceptional thermoelectric properties and intriguing anharmonic lattice dynamics underlying their low thermal conductivities. An ideal material for thermoelectric efficiency is the phonon glass–electron crystal, which drives research on strategies to scatter or localize phonons while minimally disrupting electronic-transport. Anharmonicity can potentially do both, even in perfect crystals, and simulations suggest that PbSe is anharmonic enough to support intrinsic localized modes that halt transport. Here, we experimentally observe high-temperature localization in PbSe using neutron scattering but find that localization is not limited to isolated modes – zero group velocity develops for a significant section of the transverse optic phonon on heating above a transition in the anharmonic dynamics. Arrest of the optic phonon propagation coincides with unusual sharpening of the longitudinal acoustic mode due to a loss of phase space for scattering. Our study shows how nonlinear physics beyond conventional anharmonic perturbations can fundamentally alter vibrational transport properties., To optimize the performance of lead chalcogenides for thermoelectric applications, strategies to further reduce the crystal’s thermal conductivity is required. Here, the authors discover anharmonic localized vibrations in PbSe crystals for optimizing the crystal’s vibrational transport properties.

Lead halide perovskites such as methylammonium lead triiodide (MAPI) have outstanding optical and electronic properties for photovoltaic applications, yet a full understanding of how this solution processable material works so well is currently missing. Previous research has revealed that MAPI possesses multiple forms of static disorder regardless of preparation method, which is surprising in light of its excellent performance. Using high energy resolution inelastic X-ray (HERIX) scattering, we measure phonon dispersions in MAPI and find direct evidence for another form of disorder in single crystals: large amplitude anharmonic zone-edge rotational instabilities of the PbI_6 octahedra that persist to room temperature and above, left over from structural phase transitions that take place tens to hundreds of degrees below. Phonon calculations show that the orientations of the methylammonium couple strongly and cooperatively to these modes. The result is a non-centrosymmetric, instantaneous local structure, which we observe in atomic pair distribution function (PDF) measurements. This local symmetry breaking is unobservable by Bragg diffraction, but can explain key material properties such as the structural phase sequence, ultra low thermal transport, and large minority charge carrier lifetimes despite moderate carrier mobility., 30 pages, 11 figures

Lattice dynamics and elastic constants in ${\mathrm{Mg}}_{2}{\mathrm{Si}}_{1\ensuremath{-}x}{\mathrm{Sn}}_{x}$ were investigated using resonant ultrasound spectroscopy, M\"ossbauer spectroscopy, nuclear inelastic scattering, and inelastic x-ray scattering. Increasing the Sn content $x$ results in smaller elastic constants, lower Sn specific Debye temperature, lower speed of sound, and a softening of acoustic Sn specific phonons. However, close to band convergence at about $x=0.6$, the shear modulus is well below the expected value, which suggests a pronounced connection between band convergence and lattice dynamics in this system. Based on the determined speed of sound and average phonon group velocity, the importance of optical phonons for lattice thermal conductivity is discussed, as the significant reduction in both velocities would yield an implausibly low lattice thermal conductivity of only about 60% of the experimental value. Sn specific thermodynamic quantities calculated from the Sn specific density of phonon states substantiate the general softening of lattice vibrations upon substitution of Si by Sn. A major contribution to the vibrational entropy is thus due to Sn specific vibrational modes. The generalized density of phonon states in ${\mathrm{Mg}}_{2}{\mathrm{Si}}_{1\ensuremath{-}x}{\mathrm{Sn}}_{x}$ derived from inelastic x-ray scattering for one composition shows that vibrational modes related to lightweight Mg and Si set in above 12.5 meV, whereas Sn specific modes are concentrated around 11 meV.

Author(s): He, Y; Wu, S; Song, Y; Lee, WS; Said, AH; Alatas, A; Bosak, A; Girard, A; Souliou, SM; Ruiz, A; Hepting, M; Bluschke, M; Schierle, E; Weschke, E; Lee, JS; Jang, H; Huang, H; Hashimoto, M; Lu, DH; Song, D; Yoshida, Y; Eisaki, H; Shen, ZX; Birgeneau, RJ; Yi, M; Frano, A | Abstract: We report a persistent low-energy phonon broadening around qB∼0.28 reciprocal lattice unit (r.l.u.) along the Cu-O bond direction in the high-Tc cuprate Bi2Sr2CaCu2O8+δ (Bi-2212). We show that such broadening exists both inside and outside the conventional charge-density wave (CDW) phase, via temperature-dependent measurements in both underdoped and heavily overdoped samples. Combining inelastic hard x-ray scattering, diffuse scattering, angle-resolved photoemission spectroscopy, and resonant soft x-ray scattering at the Cu L3-edge, we exclude the presence of a CDW in the heavily overdoped Bi-2212 similar to that observed in the underdoped systems. Finally, we discuss the origin of such anisotropic low-energy phonon broadening and its potential precursory role to the CDW phase in the underdoped region.

The juxtaposition of a liquid iron‐dominant alloy against a mixture of silicate and oxide minerals at Earth's core‐mantle boundary is associated with a wide range of complex seismological features. One category of observed structures is ultralow‐velocity zones, which are thought to correspond to either aggregates of partially molten material or solid, iron‐enriched assemblages. We measured the phonon dispersion relations of (Mg,Fe) O magnesiowustite containing 76 mol % FeO, a candidate ultralow‐velocity zone phase, at high pressures using high‐energy resolution inelastic X‐ray scattering. From these measurements, we find that magnesiowustite becomes strongly elastically anisotropic with increasing pressure, potentially contributing to a significant proportion of seismic anisotropy detected near the base of the mantle.

Studying the velocity–density profiles of iron and iron–silicon alloy at high pressures and temperatures is critical for understanding the Earth’s core as well as the interiors of other planetary bodies. Here we have investigated the compressional wave velocity ( V P ) and density ( ρ ) profiles of polycrystalline bcc-Fe and Fe 0.85 Si 0.15 alloy (8 wt.% Si) using in situ high-energy resolution inelastic X-ray scattering (HERIX) and synchrotron X-ray diffraction spectroscopies in an externally-heated diamond anvil cell (EHDAC) up to 15 GPa and 700 K. Based on the measured velocity–density ( V P – ρ ) and velocity–pressure ( V P – P ) relations of bcc-Fe at simultaneous high pressure and temperature ( P – T ) conditions, our results show a strong V P reduction at elevated temperatures at a constant density. Comparison of the V P – ρ profiles between the bcc-Fe and bcc-Fe 0.85 Si 0.15 alloy indicates that the alloying effect of additional 8 wt.% Si on the V P – ρ relationship of bcc-Fe is predominant via a constant density decrease of approximately 0.6 g/cm 3 (7%). Compared with the literature velocity results for bcc and hcp Fe–Si alloys, the bcc-Fe and Fe–Si alloys exhibit higher V P than their hcp phase counterparts at the given bcc–hcp transition pressures. Our results here strongly support the notion that high temperature has a strong effect on the V P of Fe and that the V P – ρ profile of Fe can be affected by structural and magnetic transitions. Analyses on literature elastic constants of the bcc Fe–Si alloys, as a function of P – T and Si content, show that the bcc phase displays extremely high V P anisotropy of 16–30% and V S splitting anisotropy of 40–90% at high temperatures, while the addition of Si further enhances the anisotropy. Due to the extremely high elastic anisotropy of the bcc Fe–Si alloy, a certain portion of the bcc Fe–Si alloy with the lattice-preferred orientation may produce V P and V S anisotropies to potentially account for the observed seismic anisotropy in the inner core.

Synchrotron radiation from third-generation high-brilliance storage rings is an ideal source for X-ray microbeams. The aim of this paper is to describe a microfocusing scheme that combines both a toroidal mirror and Kirkpatrick–Baez (KB) mirrors for upgrading the existing optical system for inelastic X-ray scattering experiments at sector 3 of the Advanced Photon Source.SHADOWray-tracing simulations without considering slope errors of both the toroidal mirror and KB mirrors show that this combination can provide a beam size of 4.5 µm (H) × 0.6 µm (V) (FWHM) at the end of the existing D-station (66 m from the source) with use of full beam transmission of up to 59%, and a beam size of 3.7 µm (H) × 0.46 µm (V) (FWHM) at the front-end of the proposed E-station (68 m from the source) with a transmission of up to 52%. A beam size of about 5 µm (H) × 1 µm (V) can be obtained, which is close to the ideal case, by using high-quality mirrors (with slope errors of less than 0.5 µrad r.m.s.). Considering the slope errors of the existing toroidal and KB mirrors (5 and 2.9 µrad r.m.s., respectively), the beam size grows to about 13.5 µm (H) × 6.3 µm (V) at the end of the D-station and to 12.0 µm (H) × 6.0 µm (V) at the front-end of the proposed E-station. The simulations presented here are compared with the experimental measurements that are significantly larger than the theoretical values even when slope error is included in the simulations. This is because of the experimental set-up that could not yet be optimized.

High-resolution inelastic X-ray scattering was used to investigate the collective vibrational excitations in hydrated lysozyme powders as a function of hydration level and temperature. It is found that the samples with strong enzymatic function are "soft", in the sense that they exhibit low frequency and large amplitude intraprotein collective vibrational motions on certain length scales. This is not the case for samples with weak or no enzymatic activity. Thus, we identify a possible correlation between the short-time intraprotein collective vibrational motions and the establishment of enzymatic function in hydrated lysozyme powders, and bring new insight to notions of protein "conformational flexibility" and "softness" in terms of these motions.

Cubic boron arsenide (BAs) was predicted to have an exceptionally high thermal conductivity $(k)\ensuremath{\sim}2000\phantom{\rule{0.16em}{0ex}}\mathrm{W}\phantom{\rule{0.16em}{0ex}}{\mathrm{m}}^{\ensuremath{-}1}{\mathrm{K}}^{\ensuremath{-}1}$ at room temperature, comparable to that of diamond, based on first-principles calculations. Subsequent experimental measurements, however, only obtained a $k$ of $\ensuremath{\sim}200\phantom{\rule{0.16em}{0ex}}\mathrm{W}\phantom{\rule{0.16em}{0ex}}{\mathrm{m}}^{\ensuremath{-}1}{\mathrm{K}}^{\ensuremath{-}1}$. To gain insight into this discrepancy, we measured phonon dispersion of single-crystal BAs along high symmetry directions using inelastic x-ray scattering and compared these with first-principles calculations. Based on the measured phonon dispersion, we have validated the theoretical prediction of a large frequency gap between acoustic and optical modes and bunching of acoustic branches, which were considered the main reasons for the predicted ultrahigh $k$. This supports its potential to be a super thermal conductor if very-high-quality single-crystal samples can be synthesized.

The competition between superconductivity and other ground states of solids is one of the challenging topics in condensed matter physics. Apart from high-temperature superconductors [1,2] this interplay also plays a central role in the layered transition-metal dichalcogenides, where superconductivity is stabilized by suppressing charge-density-wave order to zero temperature by intercalation [3] or applied pressure [4-7]. 1T-TiSe$_2$ forms a prime example, featuring superconducting domes on intercalation as well as under applied pressure. Here, we present high energy-resolution inelastic x-ray scattering measurements of the CDW soft phonon mode in intercalated Cu$_x$TiSe$_2$ and pressurized 1T-TiSe$_2$ along with detailed ab-initio calculations for the lattice dynamical properties and phonon-mediated superconductivity. We find that the intercalation-induced superconductivity can be explained by a solely phonon-mediated pairing mechanism, while this is not possible for the superconducting phase under pressure. We argue that a hybridization of phonon and exciton modes in the pairing mechanism is necessary to explain the full observed temperature-pressure-intercalation phase diagram. These results indicate that 1T-TiSe$_2$ under pressure is close to the elusive state of the excitonic insulator.

Acoustic phonons in an individual, oriented fiber of chrysotile asbestos (chemical formula Mg3Si2O5(OH)4) were observed at room temperature in the inelastic x-ray measurement with a very high (meV) resolution. The x-ray scattering vector was aligned along [1 0 0] direction of the reciprocal lattice, nearly parallel to the long axis of the fiber. The latter coincides with [1 0 0] direction of the direct lattice and the axes of the nano-channels. The data were analyzed using a damped harmonic oscillator model. Analysis of the phonon dispersion in the first Brillouin zone yielded the longitudinal sound velocity of (9200 ± 600) m / s.

In this study, collective excitations of liquid indium are studied just above the melting point at different pressures (1.7 GPa, 240 °C; 3.0 GPa, 300 °C; 4.0 GPa, 360 °C). The pressures and temperatures are achieved by the use of an externally heated diamond anvil cell. Clear evidence for the existence of propagating modes is observed from the dynamical structure factor at constant momentum transfer (Q) up to about 18 nm−1. The reason for the observed high elastic-scattering background is identified, and its effects on the determination of elastic properties such as viscosity are discussed.

Ferroelectric transitions of a hexagonal multiferroic, $\mathrm{ErMn}{\mathrm{O}}_{3}$, are studied by x-ray scattering techniques. An isosymmetry transition, similar to that previously observed for $\mathrm{YMn}{\mathrm{O}}_{3}$, approximately 300 K below the well-known ferroic transition temperature, is investigated. The partially glassy behavior of the isosymmetry transition is identified by the appearance of quasielastic scattering lines in high-energy-resolution scans. The glassy behavior is further supported by the increased interlayer decorrelation of $(\sqrt{3}\ifmmode\times\else\texttimes\fi{}\sqrt{3})R{30}^{\ensuremath{\circ}}$ ordering below the isosymmetry transition. The transition behavior is considered for possible hidden sluggish modes and two-step phase transitions theoretically predicted for the stacked triangular antiferromagnets. The in-plane azimuthal (orientational) ordering behaviors were also compared to the theoretical predictions. Coherent x-ray speckle measurements show unambiguously that the domain sizes decrease anomalously near both the isosymmetry and ferroic transitions. However, domain boundary fluctuations increase monotonically with an Arrhenius form with an activation energy of 0.54(5) eV through both transitions.

PbTe1-x Se x alloys are of special interest to thermoelectric applications. Inelastic x-ray scattering determination of phonon dispersion and lifetimes along the high symmetry directions for PbTe1-x Se x alloys are presented. By comparing with calculated results based on the virtual crystal model calculations combined with ab initio density functional theory, the validity of virtual crystal model is evaluated. The results indicate that the virtual crystal model is overall a good assumption for phonon frequencies and group velocities despite the softening of transverse acoustic phonon modes along [1 1 1] direction, while the treatment of lifetimes warrants caution. In addition, phonons remain a good description of vibrational modes in PbTe1-x Se x alloys.

Shear-aligned 40 wt% calf-thymus Na-DNA molecules in aqueous solutions are prepared in their liquid crystalline phases and studied by high resolution inelastic X-ray scattering (IXS). Measured IXS spectra are analyzed with the generalized three effective eignmode (GTEE) theory. The phonon dispersion relations along the axial direction of DNA molecules with different MgCl2 concentrations are constructed and compared. It is found that the sound speed along the axial direction of DNA molecules varies only slightly, but the phonon dampening is greatly affected with the increase amount of MgCl2 concentration. Using the GTEE theory, we are able to extract the longitudinal viscosity in the hydrodynamic limit from the Q-dependence of a fitted parameter. We make a comprehensive review of the GTEE theory and discuss detailed analyses of IXS spectra taking into account finite energy resolution of the instrument.

The dynamical structure factors of supercooled-liquid and hot-solid silicon are measured by inelastic X-ray scattering at the same temperature, 1620 K. Two significant changes in the averaged longitudinal sound velocities and in the longitudinal modulus are observed. First, we observe a different longitudinal modulus in the polycrystalline hot-solid silicon compared to the extrapolated value obtained from the single-crystal measurement. This reduction of the modulus may be a precursor of the semiconductor-to-metal transition. Second, the increase in the longitudinal modulus in the liquid upon supercooling is consistent with an increase in the degree of the directional bonding.

We summarize a series of experimental results made with the newly developed high resolution X-ray scattering (IXS) instrument on two pure lipid bilayers, including dimyristoylphosphatidylcholine (DMPC) and dilauroylphosphatidylcholine (DLPC) in both gel and liquid crystal phases, and lipid bilayers containing cholesterol. By analyzing the IXS data based on the generalized three effective eigenmode model (GTEE), we obtain dispersion relations of the high frequency density oscillations (phonons) of lipid molecules in these bilayers. We then compare the dispersion relations of pure lipid bilayers of different chain lengths among themselves and the dispersion relations of pure lipid bilayers with those of the cholesterol containing bilayers. We also compare our experimental results with collective dynamics data generated by computer molecular dynamics (MD) simulations for dipalmitoylphosphatidylcholine (DPPC) in gel phase and DMPC in liquid crystal phase.

Quasicrystals are aperiodic long-range ordered solids expected to exhibit peculiar dynamical properties. For these new intermetallic phases, previous theoretical work predicted the existence of phason dynamics and a highly structured vibrational density of states. We used the high-resolution inelastic X-ray scattering method to investigate the lattice dynamics of Al–Cu–Fe and Al–Pd–Mn quasicrystals, near the (18,29) diffraction peak situated on the fivefold axis. Phonon dispersion relations were determined for both quasicrystals. In addition to propagating acoustic modes, dispersionless (‘optic’) low-energy modes were observed.

Short wavelength collective excitations in liquid Hg at room temperature have been investigated by high-resolution inelastic X-ray scattering. Clear evidence for the existence of propagating modes was found from the S ( Q , ω ) at constant Q up to about 17 nm −1 . A positive dispersion in the Q – ω relation for these excitations was identified. This behavior is described in a simplified viscoelastic view.

We have combined a toroidal and a KB mirror system in tandem to improve the focal spot size for the momentum-resolved inelastic X-ray scattering (IXS) spectrometer at Sector 3 in APS. This combination provides a factor of 40 gain in flux density and 20 μm (H)×17 μm (V) (FWHM) in beam size at the sample position, enhancing the capability of the beamline for high-pressure measurements.

The high-resolution inelastic X-ray scattering technique has evolved rapidly at the third-generation synchrotron sources. It is now possible to measure collective excitations with 2 meV resolution. The next level of experiments may require even more stringent conditions in terms of energy resolution, sample size and environment. For example, microscopic single crystals, thin films or multilayers, confined liquids, and samples under high pressure are outside the domain of momentum resolved inelastic X-ray scattering. Inelastic nuclear resonant scattering can measure partial phonon density of states from such samples, provided that the samples contain suitable Mossbauer isotopes. Based on the experience obtained at the high-resolution X-ray scattering beamline (SRI-CAT 3-ID) of the APS, we present some new perspectives for X-ray sources, monochromators and analyzers to improve the performance of the spectrometer by an order of magnitude.

We present a new spectrometer at the Advanced Photon Source for inelastic X-ray scattering with an energy resolution of 2.2 meV at an incident energy of 21.6 keV. For monochromatization, a nested structure of one silicon channel cut and one ‘artificial’ channel cut is used in forward-scattering geometry. The energy analysis is achieved by a two-dimensional focusing silicon analyzer in backscattering geometry. In the first demonstration experiments, elastic scattering from a Plexiglas TM sample and two dispersion curves in a beryllium single crystal were measured. Based on these data sets, the performance of the new spectrometer is discussed. Published by Elsevier Science B.V.

We report high-resolution inelastic x-ray scattering measurements in the metallic liquid Li(NH3)4, which to a good approximation can be treated as a dilute alkali metal. We see a well-defined excitation out to large momentum transfers. This excitation shows a strong softening at wave vectors near the first peak in the structure factor, which occurs near twice the Fermi momentum.

Compressional wave velocity-density ( V P - ρ ) relations of candidate Fe alloys at relevant pressure-temperature conditions of the Earth’s core are critically needed to evaluate the composition, seismic signatures, and geodynamics of the planet’s remotest region. Specifically, comparison between seismic V P - ρ profiles of the core and candidate Fe alloys provides first-order information on the amount and type of potential light elements—including H, C, O, Si, and/or S—needed to compensate the density deficit of the core. To address this issue, here we have surveyed and analyzed the literature results in conjunction with newly measured V P - ρ results of hexagonal closest-packed (hcp) Fe and hcp-Fe 0.85 Si 0.15 alloy using in situ high-energy resolution inelastic X-ray scattering and X-ray diffraction. The nature of the Fe-Si alloy where Si is readily soluble in Fe represents an ideal solid-solution case to better understand the light-element alloying effects. Our results show that high temperature significantly decreases the V P of hcp-Fe at high pressures, and the Fe-Si alloy exhibits similar high-pressure V P - ρ behavior to hcp-Fe via a constant density offset. These V P - ρ data at a given temperature can be better described by an empirical power-law function with a concave behavior at higher densities than with a linear approximation. Our new datasets, together with literature results, allow us to build new V P - ρ models of Fe alloys in order to determine the chemical composition of the core. Our models show that the V P - ρ profile of Fe with 8 wt % Si at 6,000 K matches well with the Preliminary Reference Earth Model of the inner core.

Short-wavelength collective excitations in liquid mercury at room temperature have been studied by inelastic X-ray scattering. Up to Q values of about 17 nm-1, clear evidence for the existence of propagating modes was found from the shape of S(Q,ω) at constant Q. The Q–ω behaviour of these excitations is described in a simplified viscoelastic view.

In this work we present the results of an inelastic x-ray scattering experiment detailing the behavior of the transverse acoustic [110] phonon in BaFe${}_{2}$As${}_{2}$ as a function of temperature. When cooling through the structural transition temperature, the transverse acoustic phonon energy is reduced from the value at room temperature, reaching a maximum shift near inelastic momentum transfer $\stackrel{P\vec}{q}=0.1$. This softening of the lattice results in a change of the symmetry from tetragonal to orthorhombic at the same temperature as the transition to long-range antiferromagnetic order. While the lattice distortion is minor, the anisotropy in the magnetic exchange constants in pnictide parent compounds is large. We suggest mechanisms of electron-phonon coupling to describe the interaction between the lattice softening and the onset of magnetic ordering.

The low-energy phonons of two different graphite intercalation compounds (GICs) have been measured as a function of temperature using inelastic x-ray scattering (IXS). In the case of the non-superconductor BaC6, the phonons observed are significantly higher (up to 20%) in energy than those predicted by theory, in contrast to the reasonable agreement found in superconducting CaC6. Additional IXS intensity is observed below 15 meV in both BaC6 and CaC6. It has been previously suggested that this additional inelastic intensity may arise from defect or vacancy modes not predicted by theory [d'Astuto et al., Phys. Rev. B 81, 104519 (2010)]. Here it is shown that this additional intensity can arise directly from the polycrystalline nature of the available samples. Our results show that future theoretical work is required to understand the relationship between the crystal structure, the phonons, and the superconductivity in GICs.

Flexibility is an important property of porphyrins, both natural and synthetic. We applied two synchrotron-based techniques, nuclear resonance vibrational spectroscopy and inelastic X-ray scattering, to quantify this property by measuring the bulk modulus of a protein active-site mimic [chloro(octaethylporphyrinato)iron(III)] and the resilience of the iron environment. Their values are 6.95 ± 0.24 GPa and 15.4 ± 0.5 N/m, respectively.

Phonons, the quantum mechanical representation of lattice vibrations, and their coupling to the electronic degrees of freedom are important for understanding thermal and electric properties of materials. For the first time, phonons have been measured using resonant inelastic x-ray scattering (RIXS) across the Cu K-edge in cupric oxide (CuO). Analyzing these spectra using an ultra-short core-hole lifetime approximation and exact diagonalization techniques, we can explain the essential inelastic features. The relative spectral intensities are related to the electron-phonon coupling strengths., Comment: 11 pages, 3 figures

We measured phonon frequencies and linewidths in doped and undoped ${\text{BaFe}}_{2}{\text{As}}_{2}$ single crystals by inelastic x-ray scattering and compared our results with density functional theory calculations. In agreement with previous work, the calculated frequencies of some phonons depended on whether the ground state was magnetic or not and, in the former case, whether phonon wave vector was parallel or perpendicular to the magnetic ordering wave vector. The experimental results agreed better with the magnetic calculation than with zero Fe moment calculations, except the peak splitting expected due to magnetic domain twinning was not observed. Furthermore, phonon frequencies were unaffected by the breakdown of the magnetic ground state due to either doping or increased temperature. Based on these results we propose that phonons strongly couple not to the static order, but to high frequency magnetic fluctuations.

In the iron pnictides, the strong sensitivity of the iron magnetic moment to the arsenic position suggests a significant relationship between phonons and magnetism. We measured the phonon dispersion of several branches in the high-temperature tetragonal phase of CaFe{sub 2}As{sub 2} using inelastic x-ray scattering on single-crystal samples. These measurements were compared to ab initio calculations of the phonons. Spin-polarized calculations imposing the antiferromagnetic order present in the low-temperature orthorhombic phase dramatically improve agreement between theory and experiment. This is discussed in terms of the strong antiferromagnetic correlations that are known to persist in the tetragonal phase.

Inelastic x-ray scattering measurements of the phonon density of states (DOS) were performed on polycrystalline samples of pure $\ensuremath{\alpha}\text{-Pu}$ and $\ensuremath{\delta}{\text{-Pu}}_{0.98}{\text{Ga}}_{0.02}$ at room temperature. The heat capacity of $\ensuremath{\alpha}\text{-Pu}$ is well reproduced by contributions calculated from the measured phonon DOS plus conventional thermal-expansion and electronic contributions, showing that $\ensuremath{\alpha}\text{-Pu}$ is a ``well-behaved'' metal in this regard. A comparison of the phonon DOS of the two phases at room temperature showed that the vibrational entropy difference between them is only a quarter of the total entropy difference expected from known thermodynamic measurements. The missing entropy is too large to be accounted for by conventional electronic entropy and evidence from the literature rules out a contribution from spin fluctuations. Possible alternative sources for the missing entropy are discussed.

The second-order displacive phase transition in ${\text{SrTiO}}_{3}$ at ${T}_{C}\ensuremath{\sim}105\text{ }\text{K}$ has been the subject of much debate. For temperature $T$ above and near ${T}_{C}$, energy scans by neutron scattering have shown a central peak (CP) at the $R$ point in the Brillouin zone in addition to a pair of soft phonon peaks, while momentum scans by x-ray thermal diffuse scattering around the $R$ point have shown a narrow component (NC) atop a broad thermal peak caused by the soft mode. This work clarifies the relationship between the CP and NC by inelastic x-ray scattering with high energy and momentum resolutions. The CP and NC are derived from the same origin and can be attributed to defect-induced local transition above ${T}_{C}$.

Molecular dynamics simulations and neutron scattering experiments have shown that many hydrated globular proteins exhibit a universal dynamic transition at T D = 220 K, below which the biological activity of a protein sharply diminishes. We studied the phononlike low-energy excitations of two structurally very different proteins, lysozyme and bovine serum albumin, using inelastic x-ray scattering above and below T D . We found that the excitation energies of the high-Q phonons show a marked softening above T D . This suggests that the large amplitude motions of wavelengths corresponding to this specific Q range are intimately correlated with the increase of biological activities of the proteins.

Elastic neutron-scattering, inelastic x-ray scattering, specific-heat, and pressure-dependent electrical transport measurements have been made on single crystals of AuZn and Au_{0.52}Zn_{0.48} above and below their martensitic transition temperatures (T_M=64K and 45K, respectively). In each composition, elastic neutron scattering detects new commensurate Bragg peaks (modulation) appearing at Q = (1.33,0.67,0) at temperatures corresponding to each sample's T_M. Although the new Bragg peaks appear in a discontinuous manner in the Au_{0.52}Zn_{0.48} sample, they appear in a continuous manner in AuZn. Surprising us, the temperature dependence of the AuZn Bragg peak intensity and the specific-heat jump near the transition temperature are in favorable accord with a mean-field approximation. A Landau-theory-based fit to the pressure dependence of the transition temperature suggests the presence of a critical endpoint in the AuZn phase diagram located at T_M*=2.7K and p*=3.1GPa, with a quantum saturation temperature \theta_s=48.3 +/- 3.7K., Comment: 6 figures

Inelastic x-ray and neutron scattering were used to measure two matching lattice excitations on the $[01\ensuremath{\zeta}]$ zone boundary in $\ensuremath{\alpha}$-uranium. The excitations have the same polarization and reciprocal-space structure, but one has energy consistent with the thermal activation energy of the other, indicating that it creates the mode. The implied mechanism, where a mode is created by an amplitude fluctuation that mirrors the mode itself, is consistent with an intrinsically localized mode (ILM), and this is supported by thermodynamic data. The reciprocal-space structure, however, indicates a mode that is extended along its polarization direction, [010], and yet fully localized along a perpendicular direction, [001]. An enhancement of the thermal but not electrical conductivity with mode activation also suggests that these modes are more mobile than conventional ILMs. The behavior is, however, qualitatively similar to that predicted for ILMs on two-dimensional hexagonal lattices, where in-plane localization has been shown to be extended over more than ten discrete units, and the modes can be highly mobile.

We report measurements of the atomic form factor of lithium, beryllium, and aluminum single crystals at low-momentum transfers $(Q=1.6--50\phantom{\rule{0.3em}{0ex}}{\mathrm{nm}}^{\ensuremath{-}1})$ from the intensity of phonons observed by inelastic x-ray scattering. Comparing to Hartree-Fock calculations, the form factor deviates significantly in the case of lithium and beryllium around ${k}_{F}$. These deviations can be mostly understood on the basis of electron redistribution by a pseudopotential. The influence of multiple scattering due to coherent phonon scattering and possible deviations from the adiabatic approximation are also discussed.