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Fix a bounded, analytic, and simply connected domain $\Omega\subset\mathbb{R}^2.$ We show that all analytic steady states of the Euler equations with stream function $\psi$ are either radial or solve a semi-linear elliptic equation of the form $\Delta \psi = F(\psi)$ with Dirichlet boundary conditions. In particular, if $\Omega$ is not a ball, then there exists a one to one correspondence between analytic steady states of the Euler equations and analytic solutions of equations of the form $\Delta \psi = F(\psi)$ with Dirichlet boundary conditions.

We consider the transport of a passive scalar $f\in\mathbb{R}$ along a divergence-free velocity vector field $u\in\mathbb{R}^d$ on the infinite space $\mathbb{R}^d$. We give a quantitative version of the DiPerna-Lions well-posedness theory for Sobolev vector fields $u \in L_t^1W_x^{1,p}$ when $1

In this paper we prove that for all solutions of the 2d Euler equations with initial vorticity with finite Sobolev smoothness then an initial data dependent norm of the associated Lagrangian flow blows up in infinite time at least like $t^{\frac{1}{3}}$. This initial data dependent norm quantifies the exact $L^2$ decay of the Fourier transform of the solution. This adapted norm turns out to be the exact quantity that controls a low to high frequency cascade which we then show to be the quantitative phenomenon behind the Lyapunov construction by Shnirelman., Comment: 25 pages

We introduce a local-in-time existence and uniqueness class for solutions to the 2d Euler equation with unbounded vorticity. Furthermore, we show that solutions belonging to this class can develop stronger singularities in finite time, meaning that they experience finite time blow up and exit the wellposedness class. Such solutions may be continued as weak solutions (potentially non-uniquely) after the singularity. While the general dynamics of 2d Euler solutions beyond the Yudovich class will certainly not be so tame, studying such solutions gives a way to study singular phenomena in a more controlled setting.

Chirality is a ubiquitous phenomenon in which a symmetry between left- and right-handed objects is broken, examples in nature ranging from subatomic particles and molecules to living organisms. In particle physics, the weak force is responsible for the symmetry breaking and parity violation in beta decay, but in condensed matter systems interactions that lead to chirality remain poorly understood. Here, we unravel the mechanism of chiral charge density wave formation in the transition-metal dichalcogenide 1T-TiSe2. Using representation analysis, we show that charge density modulations and ionic displacements, which transform as a continuous scalar field and a vector field on a discrete lattice, respectively, follow different irreducible representations of the space group, despite the fact that they propagate with the same wave-vectors and are strongly coupled to each other. This charge-lattice symmetry frustration is resolved by further breaking of all symmetries not common to both sectors through induced lattice distortions, thus leading to chirality. Our theory is verified using Raman spectroscopy and inelastic x-ray scattering, which reveal that all but translation symmetries are broken at a level not resolved by state-of-the-art diffraction techniques., Comment: 10 pages, 3 figures, 1 table

Using high resolution tender-x-ray resonant inelastic scattering and hard-x-ray non-resonant inelastic scattering beyond the dipole limit we were able to detect electronic excitations in intermetallic UGa$_2$ that are highly atomic in nature. Analysis of the spectral lineshape reveals that the local $5f^2$ configuration characterizes the correlated nature of this ferromagnet. The orientation and directional dependence of the spectra indicate that the ground state is made of the $\Gamma_1$ singlet and/or $\Gamma_6$ doublet symmetry. With the ordered moment in the $ab$ plane, we infer that the magnetism originates from the higher lying $\Gamma_6$ doublet being mixed with the $\Gamma_1$ singlet due to inter-site exchange, qualifying UGa$_2$ to be a true quantum magnet. The ability to observe atomic excitations is crucial to resolve the on-going debate about the degree of localization versus itineracy in U intermetallics., Comment: 9 pages, 7 figures

We study logarithmic spiraling solutions to the 2d incompressible Euler equations which solve a nonlinear transport system on $\mathbb{S}$. We show that this system is locally well-posed in $L^p, p\geq 1$ as well as for atomic measures, that is logarithmic spiral vortex sheets. In particular, we realize the dynamics of logarithmic vortex sheets as the well-defined limit of logarithmic solutions which could be smooth in the angle. Furthermore, our formulation not only allows for a simple proof of existence and bifurcation for non-symmetric multi branched logarithmic spiral vortex sheets but also provides a framework for studying asymptotic stability of self-similar dynamics. We give a complete characterization of the long time behavior of logarithmic spirals. We prove global well-posedness for bounded logarithmic spirals as well as data that admit at most logarithmic singularities. This is due to the observation that the local circulation of the vorticity around the origin is a strictly monotone quantity of time. We are then able to show a dichotomy in the long time behavior, solutions either blow up (either in finite or infinite time) or completely homogenize. In particular, bounded logarithmic spirals should converge to constant steady states. For logarithmic spiral sheets, the dichotomy is shown to be even more drastic where only finite time blow up or complete homogenization of the fluid can and does occur., Comment: 24 pages, 2 figures. To appear in Journal de Ecole polytechnique - Mathematiques

We study the long-time behavior of scale-invariant solutions of the 2d Euler equation satisfying a discrete symmetry. We show that all scale-invariant solutions with bounded variation on $\mathbb{S}^1$ relax to states that are piece-wise constant with finitely many jumps. All continuous scale-invariant solutions become singular and homogenize in infinite time. On $\mathbb{R}^2$, this corresponds to generic infinite-time spiral and cusp formation. The main tool in our analysis is the discovery of a monotone quantity that measures the number of particles that are moving away from the origin. This monotonicity also applies locally to solutions of the 2d Euler equation that are $m$-fold symmetric ($m\geq 4$) and have radial limits at the point of symmetry. Our results are also applicable to the Euler equation on a large class of surfaces of revolution (like $\mathbb{S}^2$ and $\mathbb{T}^2$). Our analysis then gives generic spiraling of trajectories and infinite-time loss of regularity for globally smooth solutions on any such smooth surface, under a discrete symmetry.

Research on charge-density-wave (CDW) ordered transition-metal dichalcogenides continues to unravel new states of quantum matter correlated to the intertwined lattice and electronic degrees of freedom. Here, we report an inelastic x-ray scattering investigation of the lattice dynamics of the canonical CDW compound $2H$-TaSe$_2$ complemented by angle-resolved photoemission spectroscopy. Our results rule out the central-peak scenario for the CDW transition in $2H$-TaSe$_2$ and provide evidence for a novel precursor phase above the CDW transition temperature $T_{CDW}$. The phase at temperatures between $T^{*}\,(= 128.7\,,\rm{K})$ and $T_{CDW}\,(= 121.3\,\rm{K})$ is characterized by a fully softened phonon mode and medium-range ordered ($\xi_{corr} = 100\,\rm{\mathring{A}}- 200\,\rm{\mathring{A}})$ static CDW domains. Only $T_{CDW}$ is detectable in our photoemission experiments. Thus, $2H$-TaSe$_2$ exhibits structural before electronic static order and emphasizes the important lattice contribution to CDW transitions.

Acoustic phonons have recently been posited as playing an integral role in explaining the half-quantized thermal Hall effect in $\alpha$-RuCl$_3$. Therefore, we present much needed inelastic x-ray scattering measurements of its acoustic phonon dispersion, along with calculations using the frozen-phonon method. We also discuss a temperature study which conclusively shows a first-order structural transition to a non-$C2/m$ space group at low temperature. Together these results are an important backbone for future theoretical and experimental studies of $\alpha$-RuCl$_3$.

Phonon chirality has attracted intensive attention since it breaks the traditional cognition that phonons are linear propagating bosons. This new quasiparticle property has been extensively studied theoretically and experimentally. However, characterization of the phonon chirality throughout the full Brillouin zone is still not possible due to the lack of available experimental tools. In this work, phonon dispersion and chirality of tungsten carbide were investigated by millielectronvolt energy-resolution inelastic X-ray scattering. The atomistic calculation indicates that in-plane longitudinal and transverse acoustic phonons near K and K$^\prime$ points are circularly polarized due to the broken inversion symmetry. Anomalous inelastic X-ray scattering by these circularly polarized phonons was observed and attributed to their chirality. Our results show that inelastic X-ray scattering can be utilized to characterize phonon chirality in materials and suggest that a revision to the phonon scattering function is necessary.

In two-dimensional materials, structure difference induces the difference in phonon dispersions, leading to the anisotropy of in-plane thermal transport. Here, we report an exceptional case in layered PdSe2, where the bonding, force constants, and lattice constants are nearly-equal along the in-plane crystallographic axis directions. The phonon dispersions show significant differences between the Gamma-X and Gamma-Y directions, leading to the anisotropy of in-plane thermal conductivity with a ratio up to 1.8. Such anisotropy is not only unexpected in equilaterally structured (in-plane) materials but also comparable to the record in the non-equilaterally structured material reported to date. By combining inelastic X-ray scattering and first-principles calculations, we attribute such anisotropy to the low-energy phonons along Gamma-X, in particular, their lower group velocities and "avoided-crossing" behavior. The different bucking structures between a- (zigzag-type) and b-axis (flat-type) are mainly responsible for the unique phonon dynamics properties of PdSe2. The present results illustrate the unusual thermal conduction mechanism of the equilaterally structured materials and provide valuable insights on thermal management in electronic devices., Comment: 16 figures, 2 tables

Understanding lattice dynamics is crucial for effective thermal management in high-power electronic devices because phonons dominate thermal transport in most semiconductors. This study utilizes complementary inelastic X-ray and neutron scattering techniques and reports the temperature-dependent phonon dynamics of alpha-GaN, one of the most important third-generation power semiconductors. A prominent Matryoshka phonon dispersion is discovered with the scattering tools and confirmed by the first-principles calculations. Such Matryoshka twinning throughout the three-dimension reciprocal space is demonstrated to amplify the anharmonicity of the related phonon modes through creating abundant three-phonon scattering channels and cutting the phonon lifetime of affected modes by more than 50%. Such phonon topology effectively contributes to the reduction of the in-plane thermal transport, thus the anisotropic thermal conductivity of alpha-GaN. The results not only have significant implications for engineering the thermal performance and other phonon-related properties of alpha-GaN, but also offer valuable insights on the role of anomalous phonon topology in thermal transport of other technically important semiconductors., Comment: 34 pages, 15 figures

We utilized high-energy-resolution resonant inelastic X-ray scattering (RIXS) at both the Ta and Ni $L_3$-edges to map out element-specific particle-hole excitations in Ta$_2$NiSe$_5$ across the phase transition. Our results reveal a momentum dependent gap-like feature in the low energy spectrum, which agrees well with the band gap in element-specific joint density of states calculations based on ab initio estimates of the electronic structure in both the low temperature monoclinic and the high temperature orthorhombic structure. Below $T_c$, the RIXS energy-momentum map shows a minimal gap at the Brillouin zone center ($\sim$ 0.16 eV), confirming that Ta$_2$NiSe$_5$ possesses a direct band gap in its low temperature ground state. However, inside the gap, no signature of anticipated collective modes with an energy scale comparable to the gap size can be identified. Upon increasing the temperature to above $T_c$, whereas the gap at the zone center closes, the RIXS map at finite momenta still possesses the gross features of the low temperature map, suggesting a substantial mixing between the Ta and Ni orbits in the conduction and valence bands, which does not change substantially across the phase transition. Our experimental observations and comparison to the theoretical calculations lend further support that the phase transition and the corresponding gap opening in Ta$_2$NiSe$_5$ is largely structural by nature with possible minor contribution from the putative exciton condensate., Comment: The manuscript has been accepted by Physical Review B

We study the paralinearised weakly dispersive Burgers type equation: $$\partial_t u+T_u \partial_xu+\partial_x |D|^{\alpha-1}u=0,\ \alpha \in ]1,2[,$$ which contains the main non linear "worst interaction" terms, that is low-high interaction terms, of the usual weakly dispersive Burgers type equation: \[ \partial_t u+u\partial_x u+\partial_x |D|^{\alpha-1}u=0,\ \alpha \in ]1,2[, \] with $u_0 \in H^s({\mathbb D})$, where ${\mathbb D}={\mathbb T} \text{ or } {\mathbb R}$. Through a paradifferential complex Cole-Hopf type gauge transform we introduced in [42], we prove a new a priori estimate in $H^s({\mathbb D})$ under the control of $\left\Vert D^{2-\alpha}\left(u^2\right)\right\Vert_{L^1_tL^{\infty}_x}$, improving upon the usual hyperbolic control $\left\Vert \partial_x u\right\Vert_{L^1_tL^\infty_x}$. Thus we eliminate the "standard" wave breaking scenario in case of blow up as conjectured in [31]. For $\alpha\in ]2,3[$ we show that we can completely conjugate the paralinearised dispersive Burgers equation to a semi-linear equation of the form: $$\partial_t \left[T_{e^{iT_{p(u)}}}u\right]+ \partial_x |D|^{\alpha-1}\left[T_{e^{iT_{p(u)}}}u\right]=T_{R(u)}u,\ \alpha \in ]2,3[,$$ where $T_{p(u)}$ and $T_{R(u)}$ are paradifferential operators of order $0$ defined for $u\in L^\infty_t C^{(2-\alpha)^+}_*$., Comment: Updated version after review which closely follows the journal version to appear in Indiana University Mathematics Journal, 2022. arXiv admin note: text overlap with arXiv:2103.03576

In the first part of this paper we prove that the flow associated to a dispersive Burgers equation with a non local term of the form $|D|^{\alpha-1} \partial_x u$, $\alpha \in [1,+\infty[$ is Lipschitz from bounded sets of $H^s_0(\mathbb{T};\mathbb{R})$ to $C^0([0,T],H^{s-(2-\alpha)^+}_0(\mathbb{T};\mathbb{R}))$ for $T>0$ and $s>\lceil \frac{\alpha}{\alpha-1}\rceil-\frac{1}{2}$, where $H^s_0$ are the Sobolev spaces of functions with $0$ mean value, proving that the result obtained in [37] is optimal on the torus. The proof relies on a paradifferential generalization of a complex Cole-Hopf gauge transformation introduced by T.Tao in [43] for the Benjamin-Ono equation. For this we prove a generalization of the Baker-Campbell-Hausdorff formula for flows of hyperbolic paradifferential equations and prove the stability of the class of paradifferential operators modulo more regular remainders, under conjugation by such flows. For this we prove a new characterization of paradifferential operators in the spirit of Beals [9]. In the second part of this paper we use a paradifferential version of the previous method to prove that a re-normalization of the flow of the one dimensional periodic gravity capillary equation is Lipschitz from bounded sets of $H^s$ to $C^0([0,T],H^{s-\frac{1}{2}})$ for $T>0$ and $s>3+\frac{1}{2}$. This proves that the result obtained in [37] is optimal for the water waves system., Comment: Updated version after referee reports and review

The family of edge-sharing tri-coordinated iridates and ruthenates has emerged in recent years as a major platform for Kitaev spin liquid physics, where spins fractionalize into emergent magnetic fluxes and Majorana fermions with Dirac-like dispersions. While such exotic states are usually pre-empted by long-range magnetic order at low temperatures, signatures of Majorana fermions with long coherent times have been predicted to manifest at intermediate and higher energy scales, similar to the observation of spinons in quasi-1D spin chains. Here we present a Resonant Inelastic X-ray Scattering study of the magnetic excitations of the hyperhoneycomb iridate $\beta$-Li$_2$IrO$_3$ under a magnetic field with a record-high-resolution spectrometer. At low-temperatures, dispersing spin waves can be resolved around the predicted intertwined incommensurate spiral and field-induced zigzag orders, whose excitation energy reaches a maximum of 16meV. A 2T magnetic field softens the dispersion around ${\bf Q}=0$. The behavior of the spin waves under magnetic field is consistent with our semiclassical calculations for the ground state and the dynamical spin structure factor, which further predicts that the ensued intertwined uniform states remain robust up to very high fields (100 T). Most saliently, the low-energy magnon-like mode is superimposed by a broad continuum of excitations, centered around 35meV and extending up to 100meV. This high-energy continuum survives up to at least 300K -- well above the ordering temperature of 38K -- and gives evidence for pairs of long-lived Majorana fermions of the proximate Kitaev spin liquid., Comment: 8 pages, 4 figures

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 Sr$_{1-x}$Na$_x$Fe$_2$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 $\xi$ ~ 10 $\AA$ and a large nematic susceptibility $\chi_{\rm nem}$. The optimal-doped ($x=0.55$) sample exhibits weaker phonon softening effects, indicative of both reduced $\xi$ and $\chi_{\rm nem}$. Our results suggest short-range nematic fluctuations may favor superconductivity, placing emphasis on the nematic correlation length for understanding the iron-based superconductors.

By means of density functional theory plus dynamical mean-field theory (DFT+DMFT) calculations and resonant inelastic x-ray scattering (RIXS) experiments, we investigate the high-pressure phases of the spin-orbit-coupled $J_{\rm{eff}}=3/2$ insulator GaTa$_4$Se$_8$. Its metallic phase, derived from the Mott state by applying pressure, is found to carry $J_{\rm{eff}}=3/2$ moments. The characteristic excitation peak in the RIXS spectrum maintains its destructive quantum interference of $J_{\rm{eff}}$ at the Ta $L_2$-edge up to 10.4 GPa. Our exact diagonalization based DFT+DMFT calculations including spin-orbit coupling also reveal that the $J_{\rm{eff}}=3/2$ character can be clearly identified under high pressure. These results establish the intriguing nature of the correlated metallic magnetic phase, which represents the first confirmed example of $J_{\rm{eff}}$=3/2 moments residing in a metal. They also indicate that the pressure-induced superconductivity is likely unconventional and influenced by these $J_{\rm{eff}}=3/2$ moments. Based on a self-energy analysis, we furthermore propose the possibility of doping-induced superconductivity related to a spin-freezing crossover., Comment: 7 pages, 5 figures (additional 4 pages and 6 figures for supplemental materials)

The intermediate valence (IV) compound YbAl$_3$ exhibits nonintegral valence (Yb 4$f^{14-n_f}$ (5d6s)$^z$ where z = 2+n$_f$ = 2.75) in a moderately heavy (m* = 20-30me) ground state with a large Kondo temperature (T$_K$ ~ 500-600K). We have measured the magnetic fluctuations and the phonon spectra on single crystals of this material by time-of-flight inelastic neutron scattering (INS) and inelastic x-ray scattering (IXS). We find that at low temperature, the Kondo-scale spin fluctuations have a momentum (Q) dependence similar to that seen recently in the IV compound CePd$_3$ and which can be attributed to particle-hole excitations in a coherent itinerant 4$f$ correlated ground state. The Q-dependence disappears as the temperature is raised towards room temperature and the 4$f$ electron band states become increasingly incoherent. The measured phonons can be described adequately by a calculation based on standard DFT+$U$ density functional theory, without recourse to considering 4$f$ correlations dynamically. A low temperature magnetic peak observed in the neutron scattering at ~ 30meV shows dispersion identical to an optic phonon branch. This 4$f$/phonon resonance disappears for T > 150K. The phonons appear to remain unaffected by the resonance. We discuss several possibilities for the origin of this unusual excitation, including the idea that it arises from the large amplitude beating of the light Al atoms against the heavy Yb atoms, resulting in a dynamic 4$f$/3$p$ hybridization.

In this paper we revisit the hypothesis needed to define the "paracomposition" operator, an analogue to the classic pull-back operation in the low regularity setting, first introduced by S. Alinhac in [3]. More precisely we do so in two directions. First we drop the diffeomorphism hypothesis. Secondly we give estimates in global Sobolev and Zygmund spaces. Thus we fully generalize Bony's classic paralinearasition theorem giving sharp estimates for composition in Sobolev and Zygmund spaces. In order to prove that the new class of operations benefits of symbolic calculus properties when composed by a paradifferential operator, we discuss the pull-back of pseudodifferential and paradifferential operators which then become Fourier Integral Operators. In this discussion we show that those Fourier Integral Operators obtained by pull-back are pseudodifferential or paradifferential operators if and only if they are pulled-back by a diffeomorphism that is a change of variable. We give a proof of the change of variables in paradifferential operators. Finally we study the cutoff defining paradifferential operators and it's stability by successive composition. It is known that the cutoff becomes worse after each composition, we give a slightly refined version of the cutoffs proposed by H\"ormander in [14] for which give an optimal estimate on the support of the cutoff after composition., Comment: Updated version after referee reports and review

In the first part of this paper we prove that the flow associated to the Burgers equation with a non local term of the form $\partial_x |D|^{\alpha-1} u$ fails to be uniformly continuous from bounded sets of $H^s({\mathbb D})$ to $C^0([0,T],H^s({\mathbb D}))$ for $T>0$, $s>\frac{1}{2}+2$, $0\leq \alpha <2$, ${\mathbb D}={\mathbb R} \ \text{or} \ {\mathbb T} $. Furthermore we show that the flow cannot be $C^1$ from bounded sets of $H^s({\mathbb D})$ to $C^0([0,T],H^{s-1+(\alpha-1)^+ +\epsilon}({\mathbb D}))$ for $\epsilon>0$. We generalize this result to a large class of nonlinear transport-dispersive equations in any dimension, that in particular contains the Whitham equation and the paralinearization of the water waves system with and without surface tension. The current result is optimal in the sense that for $\alpha=2$ and ${\mathbb D}={\mathbb T}$ the flow associated to the Benjamin-Ono equation is Lipschitz on function with $0$ mean value $H^s_0$. In the second part of this paper we apply this method to deduce the quasi-linearity of the water waves system, which is the main result of this paper., Comment: Updated version after review which closely follows the journal version to appear in SIAM Journal on Mathematical Analysis, 2022

Material properties depend sensitively on the atomic arrangements and atomic bonding, but these are notoriously difficult to measure in nanosized atomic clusters due to the small size of the objects and the challenge of obtaining bulk samples of identical clusters. Here we have combined the recent ability to make gram quantities of identical semiconductor quantum-dot nanoparticles with the ability to measure lattice dynamics on small sample quantities of hydrogenated materials using high energy resolution inelastic x-ray scattering (HERIX), to measure the size-dependence of the phonon density of states (PDOS) in CdSe quantum dots. The fact that we have atomically precise structural models for these nanoparticles allows the calculation of the PDOS using Density Functional Theory (DFT), providing both experimental and theoretical confirmations of the important role that the inertia of the surface capping species plays on determining the lattice dynamics., Comment: 9 pages, 6 figures

We report a persistent low-energy phonon broadening around $q_{B} \sim 0.28$ r.l.u. along the Cu-O bond direction in the high-$T_c$ cuprate Bi$_2$Sr$_2$CaCu$_2$O$_{8+\delta}$ (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 $L_3$-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., Comment: 11 pages, 9 figures

Motivated by RIXS experiments on a wide range of complex heavy oxides, including rhenates, osmates, and iridates, we discuss the theory of RIXS for site-localized $t_{2g}$ orbital systems with strong spin-orbit coupling. For such systems, we present exact diagonalization results for the spectrum at different electron fillings, showing that it accesses "single-particle" and "multi-particle" excitations. This leads to a simple picture for the energies and intensities of the RIXS spectra in Mott insulators such as double perovskites which feature highly localized electrons, and yields estimates of the spin-orbit coupling and Hund's coupling in correlated $5d$ oxides. We present new higher resolution RIXS data at the Re-L$_3$ edge in Ba$_2$YReO$_6$ which finds a previously unresolved peak splitting, providing further confirmation of our theoretical predictions. Using ab initio electronic structure calculations on Ba$_2$${\cal M}$ReO$_6$ (with ${\cal M}$=Re, Os, Ir) we show that while the atomic limit yields a reasonable effective Hamiltonian description of the experimental observations, effects such as $t_{2g}$-$e_g$ interactions and hybridization with oxygen are important. Our ab initio estimate for the strength of the intersite exchange coupling shows that, compared to the osmates, the exchange is one or two orders of magnitude weaker in the rhenates and iridates, which may partly explain the suppression of long-range magnetic order in the latter compounds. As a way to interpolate between the site-localized picture and our electronic structure band calculations, we discuss the spin-orbital levels of the ${\cal M}$O$_6$ cluster. This suggests a possible role for non-dispersive intra-cluster excitons in Ba$_2$YIrO$_6$ which may lead to a weak breakdown of the atomic $J_{\rm eff}=0$ picture and to small magnetic moments., Comment: 11 pages, 6 figs, added experimental coauthors, revised following referee comments, published in PRB

Perovskite structured materials contain myriad tunable ordered phases of electronic and magnetic origin with proven technological importance and strong promise for a variety of energy solutions. An always-contributing influence beneath these cooperative and competing interactions is the lattice, whose physics may be obscured in complex perovskites by the many coupled degrees of freedom which makes these systems interesting. Here we report signatures of an approach to a quantum phase transition very near the ground state of the nonmagnetic, ionic insulating, simple cubic perovskite material ScF3 and show that its physical properties are strongly effected as much as 100 K above the putative transition. Spatial and temporal correlations in the high-symmetry cubic phase determined using energy- and momentum-resolved inelastic X-ray scattering as well as X-ray diffraction reveal that soft mode, central peak and thermal expansion phenomena are all strongly influenced by the transition., Comment: 6 pages, 4 figures

Recent experimental work has revealed that the unusually strong, isotropic structural negative thermal expansion in cubic perovskite ionic insulator ScF3 occurs in excited states above a ground state tuned very near a structural quantum phase transition, posing a question of fundamental interest as to whether this special circumstance is related to the anomalous behavior. To test this hypothesis, we report an elastic and inelastic X-ray scattering study of a second system Hg2I2 also tuned near a structural quantum phase transition while retaining stoichiometric composition and high crystallinity. We find similar behavior and significant negative thermal expansion below 100K for dimensions along the body-centered-tetragonal c axis, bolstering the connection between negative thermal expansion and zero temperature structural transitions. We identify the common traits between these systems and propose a set of materials design principles that can guide discovery of new materials exhibiting negative thermal expansion., Comment: 8 pages, 4 figures, accepted, Phys. Rev. Mat. 2017, 8 pages, 4 figures

Continued improvement of the energy resolution of resonant inelastic x-ray scattering (RIXS) spectrometers is crucial for fulfilling the potential of this technique in the study of electron dynamics in materials of fundamental and technological importance. In particular, RIXS is the only alternative tool to inelastic neutron scattering capable of providing fully momentum resolved information on dynamic spin structures of magnetic materials, but is limited to systems whose magnetic excitation energy scales are comparable to the energy resolution. The state-of-the-art spherical diced crystal analyzer optics provides energy resolution as good as 25 meV but has already reached its theoretical limit. Here, we demonstrate a novel sub-10meV RIXS spectrometer based on flat-crystal optics at the Ir-L$_3$ absorption edge (11.215$\sim$ keV) that achieves an analyzer energy resolution of 3.9$\sim$meV, very close to the theoretical value of 3.7$\sim$meV. In addition, the new spectrometer allows efficient polarization analysis without loss of energy resolution. The performance of the instrument is demonstrated using longitudinal acoustical and optical phonons in diamond, and magnon in Sr$_3$Ir$_2$O$_7$. The novel sub-10$\sim$meV RIXS spectrometer thus provides a window into magnetic materials with small energy scales.

Strong spin-orbit coupling lifts the degeneracy of t2g orbitals in 5d transition-metal systems, leaving a Kramers doublet and quartet with effective angular momentum of Jeff = 1/2 and 3/2, respectively. These spin-orbit entangled states can host exotic quantum phases such as topological Mott state, unconventional superconductivity, and quantum spin liquid. The lacunar spinel GaTa4Se8 was theoretically predicted to form the molecular Jeff = 3/2 ground state. Experimental verification of its existence is an important first step to exploring the consequences of the Jeff = 3/2 state. Here, we report direct experimental evidence of the Jeff = 3/2 state in GaTa4Se8 by means of excitation spectra of resonant inelastic x-rays scattering at the Ta L3 and L2 edges. We found that the excitations involving the Jeff = 1/2 molecular orbital were suppressed only at the Ta L2 edge, manifesting the realization of the molecular Jeff = 3/2 ground state in GaTa4Se8., Comment: 25 pages, 5 figures + Supplementary Materials [10 pages, 5 figures]

Organolead halide perovskites are a family of hybrid organic-inorganic compounds whose remarkable optoelectronic properties have been under intensive scrutiny in recent years. Here we use inelastic X-ray scattering to study low-energy lattice excitations in single crystals of methylammonium lead iodide and bromide perovskites. Our findings confirm the displacive nature of the cubic-to-tetragonal phase transition, which is further shown, using neutron and x-ray diffraction, to be close to a tricritical point. Lastly, we detect quasistatic symmetry-breaking nanodomains persisting well into the high-temperature cubic phase, possibly stabilized by local defects. These findings reveal key structural properties of these materials, and also bear important implications for carrier dynamics across an extended temperature range relevant for photovoltaic applications., Comment: Accepted to Physical Review B

Phonon properties of $\mathrm{Mo_3Sb_{7-x}Te_x}$ ($x=0,1.5, 1.7$), a potential high-temperature thermoelectric material, have been studied with inelastic neutron and x-ray scattering, and with first-principles simulations. The substitution of Te for Sb leads to pronounced changes in the electronic structure, local bonding, phonon density of states (DOS), dispersions, and phonon lifetimes. Alloying with tellurium shifts the Fermi level upward, near the top of the valence band, resulting in a strong suppression of electron-phonon screening, and a large overall stiffening of interatomic force-constants. The suppression in electron-phonon coupling concomitantly increases group velocities and suppresses phonon scattering rates, surpassing the effects of alloy-disorder scattering, and resulting in a surprising increased lattice thermal conductivity in the alloy. We also identify that the local bonding environment changes non-uniformly around different atoms, leading to variable perturbation strengths for different optical phonon branches. The respective roles of changes in phonon group velocities and phonon lifetimes on the lattice thermal conductivity are quantified. Our results highlight the importance of the electron-phonon coupling on phonon mean-free-paths in this compound, and also estimates the contributions from boundary scattering, umklapp scattering, and point-defect scattering., Comment: 16 pages, 13 figures

We experimentally investigate the symmetry in the Hidden Order (HO) phase of intermetallic URu2Si2 by mapping the lattice and magnetic excitations via inelastic neutron and x-ray scattering measurements in the HO and high-temperature paramagnetic phases. At all temperatures the excitations respect the zone edges of the body-centered tetragonal paramagnetic phase, showing no signs of reduced spatial symmetry, even in the HO phase. The magnetic excitations originate from transitions between hybridized bands and track the Fermi surface, whose feature are corroborated by the phonon measurements. Due to a large hybridization energy scale, a full uranium moment persists in the HO phase, consistent with a lack of observed crystal-field-split states. Our results are inconsistent with local order parameter models and the behavior of typical density waves. We suggest that an order parameter that does not break spatial symmetry would naturally explain these characteristics., Comment: 16 pages, 13 figures The scope of this work was expanded to include much more magnetic neutron scattering as well as inelastic x-ray scattering. The modes originally identified as soft phonons are magnetic. Many of the figures had their quality reduced in order to fit the arxiv file size limits. Please see the PRB article for higher quality images