arXiv subjects

R. Osborn

Publications and source records attributed to R. Osborn.

At least 19 recordsLinked to original sources

arXiv2026

Dynamic nanoscale structural correlations in strontium ruthenate

Strontium ruthenate (Sr$_2$RuO$_4$, SRO) has been the subject of intense research as a model quasi-two-dimensional metal with strong electronic correlations and potential exotic multi-component superconductor. Yet the nature of the superconducting state and its emergence remain debated, despite highly detailed knowledge of the normal-state electronic properties. Here we use diffuse neutron and x-ray scattering to uncover self-organized structural fluctuations on the picosecond timescale in SRO. We show that these nanoscale correlations do not originate from extrinsic disorder but rather involve cooperative displacements of oxygen atoms in the quintessential RuO$_2$ planes. Moreover, the observed displacement pattern is consistent with distortions due to incipient orbital order that we obtain in first-principles calculations, which suggests that orbital effects could play a pivotal role in the physics of SRO. Similar dynamic correlations may play a role in the physical properties of a wide range of prominent oxides with closely-related lamellar structures, such as the cuprates and nickelates.

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arXiv2025

Evidence for rare-region physics in the structural and electronic degrees of freedom of the nickelate La$_{2-x}$Sr$_x$NiO$_4$

We present a diffuse neutron and x-ray scattering study of structural as well as spin- and charge-density-wave fluctuations in the electrical insulator La$_{2-x}$Sr$_x$NiO$_4$. This lamellar nickelate is an isostructural analogue of the high-temperature cuprate superconductor La$_{2-x}$Sr$_x$CuO$_4$, for which recent experiments uncovered evidence for unusual structural and superconducting fluctuations indicative of rare-region physics due to inherent inhomogeneity unrelated to common point disorder effects. We find closely analogous nanoscale orthorhombic fluctuation behavior in La$_{2-x}$Sr$_x$NiO$_4$, including exponential scaling of the diffuse scattering intensity and power-law scaling of the characteristic length with relative temperature. Moreover, our neutron and x-ray scattering data reveal similar behavior for short-range magnetic and charge fluctuations above the respective ordering temperatures. These observations indicate that rare-region effects are a generic feature of perovskite-related structures and lead to universal fluctuations of both structural and electronic degrees of freedom over extended temperature ranges.

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arXiv2025

Pervasive symmetry-lowering nanoscale structural fluctuations in the cuprate La$_{2-x}$Sr$_{x}$CuO$_{4}$

The cuprate superconductors are among the most widely studied quantum materials, yet there remain fundamental open questions regarding their electronic properties and the role of the structural degrees of freedom. Recent neutron and x-ray scattering measurements uncovered exponential scaling with temperature of the strength of orthorhombic fluctuations in the tetragonal phase of $La_{2-x}Sr_xCuO_4$ and $Tl_2Ba_2CuO_{6+y}$, unusual behavior that closely resembles prior results for the emergence of superconducting fluctuations, and that points to a common origin rooted in inherent correlated structural inhomogeneity. Here we extend the measurements of $La_{2-x}Sr_xCuO_4$ to higher temperatures in the parent compound (x=0) and to optimal doping (x=0.155), and we furthermore investigate the effects of in-situ in-plane uniaxial stress. Our neutron scattering result for undoped $La_2CuO_4$ complement prior x-ray data and reveal that the structural fluctuations persist to the maximum experimental temperature of nearly 1000K, i.e., to a significant fraction of the melting point. At this temperature, the spatial correlation length extracted from the momentum-space data is still about three lattice constants. The neutron scattering experiment enables quasistatic discrimination and reveals that the response is increasingly dynamic at higher temperatures. We also find that uniaxial stress up to 500 MPa along the tetragonal [110] direction, which corresponds to a strain of about 0.2%, does not significantly alter this robust behavior. Overall, these results support the notion that subtle, underlying inhomogeneity underpins the cuprate phase diagram. Finally, we uncover (for x=0.2) low-energy structural fluctuations at a nominally forbidden reflection. While the origin of these fluctuations is not clear, they might be related to the presence of extended defects such as dislocations or stacking faults.

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arXiv2023

Stacking disorder in $\alpha$-RuCl$_3$ via x-ray three-dimensional difference pair distribution function analysis

The van der Waals layered magnet $\alpha$-RuCl$_3$ offers tantalizing prospects for the realization of Majorana quasiparticles. Efforts to understand this are, however, hampered by inconsistent magnetic and thermal transport properties likely coming from the formation of structural disorder during crystal growth, postgrowth processing, or upon cooling through the first order structural transition. Here, we investigate structural disorder in $\alpha$-RuCl$_3$ using x-ray diffuse scattering and three-dimensional difference pair distribution function (3D-$\Delta$PDF) analysis. We develop a quantitative model that describes disorder in $\alpha$-RuCl$_3$ in terms of rotational twinning and intermixing of the high and low-temperature structural layer stacking. This disorder may be important to consider when investigating the detailed magnetic and electronic properties of this widely studied material.

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arXiv2023

Two-Dimensional Short-Range Chemical Ordering in Ba1-xNaxFe2As2

A true understanding of the properties of pnictide superconductors require the development of high-quality materials and performing measurements designed to unravel their intrinsic properties and short-range nematic correlations which are often obscured by extrinsic effects such as poor crystallinity, inhomogeneity, domain formation and twinning. In this paper, we report the systematic growth of high-quality Na-substituted BaFe2As2 single crystals and their characterization using pulsed-magnetic fields x-ray diffraction and x-ray diffuse scattering. Analysis of the properties and compositions of the highest quality crystals show that their actual Na stoichiometry is about 50-60% of the nominal content and that the targeted production of crystals with specific compositions is accessible. We derived a reliable equation to estimate the Na stoichiometry based on the measured superconducting TC of these materials. Attempting to force spin reorientation and induce tetragonality, orthorhombic Ba1-xNaxFe2As2 single crystals subjected to out-of-plane magnetic fields up to 31.4T are found to exhibit strong in-plane magnetic anisotropy demonstrated by the insufficiency of such high fields in manipulating the relative population of their twinned domains or in suppressing the orthorhombic order. Broad x-ray diffuse intensity rods observed at temperatures between 30 K and 300 K uncover short-range structural correlations. Local structure modeling together with 3D-{\Delta}PDF mapping of real-space interatomic vectors show that the diffuse scattering arises from in-plane short-range chemical correlations of the Ba and Na atoms coupled with short-range atomic displacements within the same plane due to an effective size difference between the two atomic species.

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arXiv2022

Structure of Charge Density Waves in La$_{1.875}$Ba$_{0.125}$CuO$_4$

Although charge-density wave (CDW) correlations exist in several families of cuprate supercon-ductors, they exhibit substantial variation in CDW wavevector and correlation length, indicating a key role for CDW-lattice interactions. We investigated this interaction in La$_{1.875}$Ba$_{0.125}$CuO$_4$ using single crystal x-ray diffraction to collect a large number of CDW peak intensities, and determined the Cu and La/Ba atomic distortions induced by the formation of CDW order. Within the CuO$_2$ planes, the distortions involve a periodic modulation of the Cu-Cu spacing along the direction of the ordering wave vector. The charge ordering within the copper-oxygen layer induces an out-of-plane breathing modulation of the surrounding lanthanum layers, which leads to a related distortion on the adjacent copper-oxygen layer. Our result implies that the CDW-related structural distortions do not remain confined to a single layer but rather propagate an appreciable distance through the crystal. This leads to overlapping structural modulations, in which CuO$_2$ planes exhibit distortions arising from the orthogonal CDWs in adjacent layers as well as distortions from the CDW within the layer itself. We attribute this striking effect to the weak c-axis charge screening in cuprates and suggest this effect could help couple the CDW between adjacent planes in the crystal.

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arXiv2022

Local inversion-symmetry breaking in a bismuthate high-$T_c$ superconductor

The doped perovskite BaBiO$_3$ exhibits a maximum superconducting transition temperature ($T_c$) of 34 K and was the first high-$T_c$ oxide to be discovered, yet pivotal questions regarding the nature of both the metallic and superconducting states remain unresolved. Although it is generally thought that superconductivity in the bismuthates is of the conventional s-wave type, the pairing mechanism is still debated, with strong electron-phonon coupling and bismuth valence or bond disproportionation possibly playing a role. Here we use diffuse x-ray scattering and Monte Carlo modeling to study the local structure of Ba$_{1-x}$K$_x$BiO$_3$ across its insulator-metal boundary. We find no evidence for either long- or short-range disproportionation, which resolves a major conundrum, as disproportionation and the related polaronic effects are likely not relevant for the metallic and superconducting states. Instead, we uncover nanoscale structural correlations that break inversion symmetry, which has far-reaching implications for the electronic physics, including the pairing mechanism. This unexpected finding furthermore establishes that the bismuthates belong to the broader classes of materials with hidden spin-orbit coupling and a tendency towards inversion-breaking displacements.

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arXiv2021

Unconventional short-range structural fluctuations in cuprate high-$T_c$ superconductors

The interplay between structural and electronic degrees of freedom in complex materials is the subject of extensive debate in physics and materials science. Particularly interesting questions pertain to the nature and extent of pre-transitional short-range order in diverse systems ranging from shape-memory alloys to unconventional superconductors, and how this microstructure affects macroscopic properties. Here we use neutron and X-ray diffuse scattering to uncover universal structural fluctuations in La$_{2-x}$Sr$_x$CuO$_4$ and Tl$_2$Ba$_2$CuO$_{6+\delta}$, two cuprate superconductors with distinct point disorder effects and optimal superconducting transition temperatures. The fluctuations are present in wide doping and temperature ranges, including compositions that maintain high average structural symmetry, and they exhibit unusual, yet simple scaling behavior. The scaling regime is robust and universal, similar to the well-known critical fluctuations close to second-order phase transitions, but with a distinctly different physical origin. We relate this behavior to pre-transitional phenomena in a broad class of systems with structural and magnetic transitions, and propose an explanation based on rare structural fluctuations caused by intrinsic nanoscale inhomogeneity. We also uncover parallels with superconducting fluctuations, which indicates that the underlying inhomogeneity plays an important role in cuprate physics.

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arXiv2020

Ferroelectric quantum criticality and enhanced superconductivity in plastically deformed strontium titanate

The properties of quantum materials are commonly tuned using experimental variables such as pressure, magnetic field and doping. Here we explore a different approach: irreversible, plastic deformation of single crystals. We show for the superconductor SrTiO$_3$ that compressive plastic deformation induces low-dimensional superconductivity significantly above the superconducting transition temperature ($T_c$) of undeformed samples, with evidence of superconducting correlations at temperatures two orders of magnitude above the bulk $T_c$. The superconductivity enhancement is correlated with the appearance of self-organized dislocation structures, as revealed by diffuse neutron and X-ray scattering. We also observe signatures of deformation-induced quantum-critical ferroelectric fluctuations and inhomogeneous ferroelectric order via Raman scattering. These results suggest that the strain surrounding the self-organized dislocation structures induces local ferroelectricity and quantum-critical dynamics that strongly influence $T_c$, consistent with a theory of superconductivity enhanced by soft polar fluctuations. More broadly, our results demonstrate the promise of plastic deformation and dislocation engineering as tools to manipulate electronic properties of quantum materials.

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arXiv2020

Intertwined density waves in a metallic nickelate

Nickelates are a rich class of materials, ranging from insulating magnets to superconductors. But for stoichiometric materials, insulating behavior is the norm, as for most late transition metal oxides. Notable exceptions are the 3D perovskite LaNiO$_3$, an unconventional paramagnetic metal, and the layered Ruddlesden-Popper phases R$_4$Ni$_3$O$_{10}$, (R=La, Pr, Nd). The latter are particularly intriguing because they exhibit an unusual metal-to-metal transition. Here, we demonstrate that this transition results from an incommensurate density wave with both charge and magnetic character that lies intermediate in behavior between the metallic density wave seen in chromium metal and the insulating stripes typically found in layered nickelates. As such, R$_4$Ni$_3$O$_{10}$, which appears to be the first known example of an itinerant spin density wave in a 3d transition metal oxide, represents an important bridge between the paramagnetism of 3D metallic LaNiO$_3$ at higher nickel valence and the polaronic behavior of quasi-2D R$_{2-x}$Sr$_x$NiO$_4$ at lower nickel valence.

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arXiv2016

Detailed magnetic and structural analysis mapping a robust magnetic C4 dome in Sr1-xNaxFe2As2

The recently discovered $C_4$ tetragonal magnetic phase in hole-doped members of the iron-based superconductors provides new insights into the origin of unconventional superconductivity. Previously observed in Ba$_{1-x}A_x$Fe$_2$As$_2$ (with $A =$ K, Na), the $C_4$ magnetic phase exists within the well studied $C_2$ spin-density wave (SDW) dome, arising just before the complete suppression of antiferromagnetic (AFM) order but after the onset of superconductivity. Here, we present detailed x-ray and neutron diffraction studies of Sr$_{1-x}$Na$_x$Fe$_2$As$_2$ ($0.10 \leq\ x \leq\ 0.60$) to determine their structural evolution and the extent of the $C_4$ phase. Spanning $Δx\sim 0.14$ in composition, the $C_4$ phase is found to extend over a larger range of compositions, and to exhibit a significantly higher transition temperature, $T_r \sim 65$K, than in either of the other systems in which it has been observed. The onset of this phase is seen near a composition ($x \sim 0.30$) where the bonding angles of the Fe$_2$As$_2$ layers approach the perfect $109.46^\circ$ tetrahedral angle. We discuss the possible role of this return to a higher symmetry environment for the magnetic iron site in triggering the magnetic reorientation and the coupled re-entrance to the tetragonal structure. Finally, we present a new phase diagram, complete with the $C_4$ phase, and use its observation in a third hole-doped 122 system to suggest the universality of this phase.

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arXiv2015

Emergence of coherence in the charge-density wave state of 2H-NbSe$_2$

A charge-density wave (CDW) state has a broken symmetry described by a complex order parameter with an amplitude and a phase. The conventional view, based on clean, weak-coupling systems, is that a finite amplitude and long-range phase coherence set in simultaneously at the CDW transition temperature T$_{cdw}$. Here we investigate, using photoemission, X-ray scattering and scanning tunneling microscopy, the canonical CDW compound 2H-NbSe$_2$ intercalated with Mn and Co, and show that the conventional view is untenable. We find that, either at high temperature or at large intercalation, CDW order becomes short-ranged with a well-defined amplitude that impacts the electronic dispersion, giving rise to an energy gap. The phase transition at T$_{cdw}$ marks the onset of long-range order with global phase coherence, leading to sharp electronic excitations. Our observations emphasize the importance of phase fluctuations in strongly coupled CDW systems and provide insights into the significance of phase incoherence in `pseudogap' states.

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arXiv2015

Double-Q spin-density wave in iron arsenide superconductors

Elucidating the nature of the magnetic ground state of iron-based superconductors is of paramount importance in unveiling the mechanism behind their high temperature superconductivity. Until recently, it was thought that superconductivity emerges only from an orthorhombic antiferromagnetic stripe phase, which can in principle be described in terms of either localized or itinerant spins. However, we recently reported that tetragonal symmetry is restored inside the magnetically ordered state of a hole-doped BaFe2As2. This observation was interpreted as indirect evidence of a new double-Q magnetic structure, but alternative models of orbital order could not be ruled out. Here, we present Mossbauer data that show unambiguously that half of the iron sites in this tetragonal phase are non-magnetic, establishing conclusively the existence of a novel magnetic ground state with a non-uniform magnetization that is inconsistent with localized spins. We show that this state is naturally explained as the interference between two spin-density waves, demonstrating the itinerant character of the magnetism of these materials and the primary role played by magnetic over orbital degrees of freedom.

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arXiv2014

Symmetry of re-entrant tetragonal phase in Ba1-xNaxFe2As2: Magnetic versus orbital ordering mechanism

Magneto-structural phase transitions in Ba1-xAxFe2As2 (A = K, Na) materials are discussed for both magnetically and orbitally driven mechanisms, using a symmetry analysis formulated within the Landau theory of phase transitions. Both mechanisms predict identical orthorhombic space-group symmetries for the nematic and magnetic phases observed over much of the phase diagram, but they predict different tetragonal space-group symmetries for the newly discovered re-entrant tetragonal phase in Ba1-xNaxFe2As2 (x ~ 0.24-0.28). In a magnetic scenario, magnetic order with moments along the c-axis, as found experimentally, does not allow any type of orbital order, but in an orbital scenario, we have determined two possible orbital patterns, specified by P4/mnc1' and I4221' space groups, which do not require atomic displacements relative to the parent I4/mmm1' symmetry and, in consequence, are indistinguishable in conventional diffraction experiments. We demonstrate that the three possible space groups are however, distinct in resonant X-ray Bragg diffraction patterns created by Templeton & Templeton scattering. This provides an experimental method of distinguishing between magnetic and orbital models.

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arXiv2014

Q-dependence of the spin fluctuations in the intermediate valence compound CePd3

We report inelastic neutron scattering experiments on a single crystal of the intermediate valence compound CePd3. At 300 K the magnetic scattering is quasielastic, with halfwidth of 23 meV, and is independent of momentum transfer Q. At low temperature, the Q-averaged magnetic spectrum is inelastic, exhibiting a broad peak centered near Emax = 55 meV. These results, together with the temperature dependence of the susceptibility, 4f occupation number, and specific heat, can be fit by the Kondo/Anderson impurity model. The low temperature scattering near Emax, however, shows significant variations with Q, reflecting the coherence of the 4f lattice. The intensity is maximal at (1/2, 1/2,0), intermediate at (1/2,0,0) and (0,0,0), and weak at (1/2,1/2,1/2). We discuss this Q-dependence in terms of current ideas about coherence in heavy fermion systems.

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arXiv2013

Optic phonons and the soft mode in 2H-NbSe2

We present an investigation of the lattice dynamics of the charge-density-wave compound 2H-NbSe2. We analyze the precise nature of the wave vector dependent electron-phonon coupling (EPC) and derive the bare dispersion of the charge-density-wave (CDW) soft phonon mode using inelastic x-ray scattering combined with ab-initio calculations. Experimentally, phonon modes along the Γ - M line, i.e. q = (h, 0, 0) with 0 <= h <= 0.5, with the same longitudinal symmetry (Σ1) as the CDW soft mode were investigated up to 32 meV. In agreement with our calculations we observe significant EPC in the optic modes at h <= 0.2. We analyze the EPC in the optic as well as acoustic modes and show that the q dependences stem from scattering processes between two bands at the Fermi surface both having Nb 4d character. Finally, we demonstrate that the soft mode dispersion at T = 33 K (= {T_{CDW}}) can be well described on the basis of a strongly q dependent EPC matrix element and an acoustic-like bare phonon dispersion in agreement with observations near room temperature.

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arXiv2012

Electron-phonon coupling in the conventional superconductor YNi$_2$B$_2$C at high phonon energies studied by time-of-flight neutron spectroscopy

We report an inelastic neutron scattering investigation of phonons with energies up to 159 meV in the conventional superconductor YNi$_2$B$_2$C. Using the SWEEP mode, a newly developed time-of-flight technique involving the continuous rotation of a single crystal specimen, allowed us to measure a four dimensional volume in (Q,E) space and, thus, determine the dispersion surface and linewidths of the $A_{1g}$ (~ 102 meV) and $A_u$ (~ 159 meV) type phonon modes for the whole Brillouin zone. Despite of having linewidths of $Γ= 10 meV$, $A_{1g}$ modes do not strongly contribute to the total electron-phonon coupling constant $λ$. However, experimental linewidths show a remarkable agreement with ab-initio calculations over the complete phonon energy range demonstrating the accuracy of such calculations in a rare comparison to a comprehensive experimental data set.

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arXiv2011

Response of acoustic phonons to charge and orbital order in the 50\% doped bilayer manganite LaSr$_2$Mn$_2$O$_7$

We report an inelastic neutron scattering study of acoustic phonons in the charge and orbitally ordered bilayer manganite LaSr$_2$Mn$_2$O$_7$. For excitation energies less than $15\,\rm{meV}$, we observe an abrupt increase (decrease) of the phonon energies (linewidths) of a transverse acoustic phonon branch at $\mathbf{q} = (h, h, 0)$, $h\le0.3$, upon entering the low temperature charge and orbital ordered state ($T_{COO} = 225\,\rm{K}$). This indicates a reduced electron-phonon coupling due to a decrease of electronic states at the Fermi level leading to a partial removal of the Fermi surface below $T_{COO}$ and provides direct experimental evidence for a link between electron-phonon coupling and charge order in manganites.

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