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    Direct Observation of Shock-Induced Disordering of Enstatite Below the Melting Temperature
    (Hoboken, NJ [u.a.] : Wiley, 2020) Hernandez, J.-A.; Morard, G.; Guarguaglini, M.; Alonso-Mori, R.; Benuzzi-Mounaix, A.; Bolis, R.; Fiquet, G.; Galtier, E.; Gleason, A.E.; Glenzer, S.; Guyot, F.; Ko, B.; Lee, H.J.; Mao, W.L.; Nagler, B.; Ozaki, N.; Schuster, A.K.; Shim, S.H.; Vinci, T.; Ravasio, A.
    We report in situ structural measurements of shock-compressed single crystal orthoenstatite up to 337 ± 55 GPa on the Hugoniot, obtained by coupling ultrafast X-ray diffraction to laser-driven shock compression. Shock compression induces a disordering of the crystalline structure evidenced by the appearance of a diffuse X-ray diffraction signal at nanosecond timescales at 80 ± 13 GPa on the Hugoniot, well below the equilibrium melting pressure (>170 GPa). The formation of bridgmanite and post-perovskite have been indirectly reported in microsecond-scale plate-impact experiments. Therefore, we interpret the high-pressure disordered state we observed at nanosecond scale as an intermediate structure from which bridgmanite and post-perovskite crystallize at longer timescales. This evidence of a disordered structure of MgSiO3 on the Hugoniot indicates that the degree of polymerization of silicates is a key parameter to constrain the actual thermodynamics of shocks in natural environments. © 2020. The Authors.
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    Hidden Charge Order in an Iron Oxide Square-Lattice Compound
    (College Park, Md. : APS, 2021) Kim, Jung-Hwa; Peets, Darren C.; Reehuis, Manfred; Adler, Peter; Maljuk, Andrey; Ritschel, Tobias; Allison, Morgan C.; Geck, Jochen; Mardegan, Jose R. L.; Bereciartua Perez, Pablo J.; Francoual, Sonia; Walters, Andrew C.; Keller, Thomas; Abdala, Paula M.; Pattison, Philip; Dosanjh, Pinder; Keimer, Bernhard
    Since the discovery of charge disproportionation in the FeO2 square-lattice compound Sr3Fe2O7 by Mössbauer spectroscopy more than fifty years ago, the spatial ordering pattern of the disproportionated charges has remained “hidden” to conventional diffraction probes, despite numerous x-ray and neutron scattering studies. We have used neutron Larmor diffraction and Fe K-edge resonant x-ray scattering to demonstrate checkerboard charge order in the FeO2 planes that vanishes at a sharp second-order phase transition upon heating above 332 K. Stacking disorder of the checkerboard pattern due to frustrated interlayer interactions broadens the corresponding superstructure reflections and greatly reduces their amplitude, thus explaining the difficulty of detecting them by conventional probes. We discuss the implications of these findings for research on “hidden order” in other materials.
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    A neutron diffraction study of crystal and low-temperature magnetic structures within the (Na,Li)FeGe2O6 pyroxene-type solid solution series
    (Berlin ; Heidelberg : Springer, 2017-5-12) Redhammer, Günther J.; Senyshyn, Anatoliy; Lebernegg, Stefan; Tippelt, Gerold; Dachs, Edgar; Roth, Georg
    Solid solution compounds along the Li1–x Na x FeGe2O6 clinopyroxene series have been prepared by solid state ceramic sintering and investigated by bulk magnetic and calorimetric methods; the Na-rich samples with x(Na) > 0.7 were also investigated by low-temperature neutron diffraction experiments in a temperature range of 4–20 K. For samples with x(Na) > 0.76 the crystal structure adopts the C2/c symmetry at all measuring temperatures, while the samples display P21/c symmetry for smaller Na contents. Magnetic ordering is observed for all samples below 20 K with a slight decrease of T N with increasing Na content. The magnetic spin structures change distinctly as a function of chemical composition: up to x(Na) = 0.72 the magnetic structure can be described by a commensurate arrangement of magnetic spins with propagation vector k = (½, 0 0), an antiferromagnetic (AFM) coupling within the Fe3+O6 octahedra zig-zag chains and an alternating AFM and ferromagnetic (FM) interaction between the chains, depending on the nature of the tetrahedral GeO4 chains. The magnetic structure can be described in magnetic space group P a21/c. Close to the structural phase transition for sample with x(Na) = 0.75, magnetic ordering is observed below 15 K; however, it becomes incommensurately modulated with k = (0.344, 0, 0.063). At 4 K, the magnetic spin structure best can be described by a cycloidal arrangement within the M1 chains, the spins are within the a–c plane. Around 12 K the cycloidal structure transforms to a spin density wave (SDW) structure. For the C2/c structures, a coexistence of a simple collinear and an incommensurately modulated structure is observed down to lowest temperatures. For 0.78 ≤ x(Na) ≤ 0.82, a collinear magnetic structure with k = (0 1 0), space group P C21/c and an AFM spin structure within the M1 chains and an FM one between the spins is dominating, while the incommensurately modulated structure becomes dominating the collinear one in the samples with x(Na) = 0.88. Here the magnetic propagation vector is k = (0.28, 1, 0.07) and the spin structure corresponds again to a cycloidal structure within the M1 chains. As for the other samples, a transition from the cycloidal to a SDW structure is observed. Based on the neutron diffraction data, the appearance of two peaks in the heat capacity of Na-rich samples can now be interpreted as a transition from a cycloidal magnetic structure to a spin density wave structure of the magnetically ordered phase for the Na-rich part of the solid solution series.
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    Measurement of Spin Dynamics in a Layered Nickelate Using X-Ray Photon Correlation Spectroscopy: Evidence for Intrinsic Destabilization of Incommensurate Stripes at Low Temperatures
    (College Park, Md. : APS, 2021) Ricci, Alessandro; Poccia, Nicola; Campi, Gaetano; Mishra, Shrawan; Müller, Leonard; Joseph, Boby; Shi, Bo; Zozulya, Alexey; Buchholz, Marcel; Trabant, Christoph; Lee, James C. T.; Viefhaus, Jens; Goedkoop, Jeroen B.; Nugroho, Agustinus Agung; Braden, Markus; Roy, Sujoy; Sprung, Michael; Schüßler-Langeheine, Christian
    We study the temporal stability of stripe-type spin order in a layered nickelate with x-ray photon correlation spectroscopy and observe fluctuations on timescales of tens of minutes over a wide temperature range. These fluctuations show an anomalous temperature dependence: they slow down at intermediate temperatures and speed up on both heating and cooling. This behavior appears to be directly connected with spatial correlations: stripes fluctuate slowly when stripe correlation lengths are large and become faster when spatial correlations decrease. A low-temperature decay of nickelate stripe correlations, reminiscent of what occurs in cuprates as a result of a competition between stripes and superconductivity, hence occurs via loss of both spatial and temporal correlations.
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    Coexistence of Superconductivity and Charge Density Waves in Tantalum Disulfide : Experiment and Theory
    (College Park, Md. : APS, 2020) Kvashnin, Y.; VanGennep, D.; Mito, M.; Medvedev, S.A.; Thiyagarajan, R.; Karis, O.; Vasiliev, A.N.; Eriksson, O.; Abdel-Hafiez, M.
    The coexistence of charge density wave (CDW) and superconductivity in tantalum disulfide (2H-TaS2) at low temperature is boosted by applying hydrostatic pressures to study both vibrational and magnetic transport properties. Around Pc, we observe a superconducting dome with a maximum superconducting transition temperature Tc=9.1 K. First-principles calculations of the electronic structure predict that, under ambient conditions, the undistorted structure is characterized by a phonon instability at finite momentum close to the experimental CDW wave vector. Upon compression, this instability is found to disappear, indicating the suppression of CDW order. The calculations reveal an electronic topological transition (ETT), which occurs before the suppression of the phonon instability, suggesting that the ETT alone is not directly causing the structural change in the system. The temperature dependence of the first vortex penetration field has been experimentally obtained by two independent methods. While a d wave and single-gap BCS prediction cannot describe the lower critical field Hc1 data, the temperature dependence of the Hc1 can be well described by a single-gap anisotropic s-wave order parameter. © 2020 authors. Published by the American Physical Society.
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    Unraveling the Orbital Physics in a Canonical Orbital System KCuF3
    (College Park, Md. : APS, 2021) Li, Jiemin; Xu, Lei; Garcia-Fernandez, Mirian; Nag, Abhishek; Robarts, H.C.; Walters, A.C.; Liu, X.; Zhou, Jianshi; Wohlfeld, Krzysztof; van den Brink, Jeroen; Ding, Hong; Zhou, Ke-Jin
    We explore the existence of the collective orbital excitations, orbitons, in the canonical orbital system KCuF3 using the Cu L3-edge resonant inelastic x-ray scattering. We show that the nondispersive high-energy peaks result from the Cu2+  dd orbital excitations. These high-energy modes display good agreement with the ab initio quantum chemistry calculation, indicating that the dd excitations are highly localized. At the same time, the low-energy excitations present clear dispersion. They match extremely well with the two-spinon continuum following the comparison with Müller ansatz calculations. The localized dd excitations and the observation of the strongly dispersive magnetic excitations suggest that the orbiton dispersion is below the resolution detection limit. Our results can reconcile with the strong local Jahn-Teller effect in KCuF3, which predominantly drives orbital ordering.