Structural and magnetic aspects of the nanotube system Na2xV3O7

O. Zaharko, J. L. Gavilano, Th. Strässle, C. F. Miclea, A. C. Mota, Y. Filinchuk, D. Chernyshov, P. P. Deen, B. Rahaman, T. Saha-Dasgupta, R. Valentí, Y. Matsushita, A. Dönni, and H. Kitazawa
Phys. Rev. B 78, 214426 – Published 18 December 2008
Abstract
Authors
Article Text
  • INTRODUCTION
  • EXPERIMENTAL DETAILS
  • RESULTS
  • AB INITIO DFT CALCULATIONS
  • SUMMARY
  • ACKNOWLEDGEMENTS
  • References

    Abstract

    We present experimental results of low-temperature x-ray synchrotron diffraction, neutron-scattering, and very low-temperature (mK range) bulk measurements on the nanotube system Na2V3O7. The crystal structure determined from our data is similar to the previously proposed model [P. Millet et al., J. Solid State Chem. 147, 676 (1999)], but also deviates from it in significant details. The structure comprises of nanotubes along the c axis formed by stacking units of two V rings buckled in the ab plane. The space group is P3 ̄ and the composition is nonstoichiometric, Na2xV3O7, x=0.17. The thermal evolution of the lattice parameters reveals anisotropic lattice compression on cooling. Neutron-scattering experiments monitor a very weak magnetic signal at energies from 20 to 9 meV. Magnetic susceptibility, specific-heat measurements, and decay of remanent magnetization in the 30–300 mK range reveal that the previously observed transition at 76mK is spin-glass like with no long-range order. Presented experimental observations do not support models of isolated clusters but are compatible with a model of odd-legged S=1/2 spin tubes possibly segmented into fragments with different lengths.

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    • Received 27 August 2008

    DOI:https://doi.org/10.1103/PhysRevB.78.214426

    ©2008 American Physical Society

    Authors & Affiliations

    O. Zaharko *, J. L. Gavilano, and Th. Strässle

    • Laboratory for Neutron Scattering, ETH Zurich & Paul Scherrer Institut, CH-5232 Villigen, Switzerland

    C. F. Miclea

    • Max-Planck-Institute for Chemical Physics of Solids (MPICPfS), D-01187 Dresden, Germany

    A. C. Mota

    • Laboratory for Solid State Physics, ETH-Hönggerberg, CH-8093 Zürich, Switzerland and Max-Planck-Institute for Chemical Physics of Solids (MPICPfS), D-01187 Dresden, Germany

    Y. Filinchuk and D. Chernyshov

    • Swiss-Norwegian Beamlines, ESRF, F-38042 Grenoble Cedex 9, France

    P. P. Deen

    • Institut Laue-Langevin, 156X, F-38042 Grenoble Cedex 9, France

    B. Rahaman and T. Saha-Dasgupta

    • S.N. Bose National Centre for Basic Sciences, JD Block, Sector 3, Salt Lake City, Kolkata 700098, India

    R. Valentí

    • Institute of Theoretical Physics, University of Frankfurt, D-60438 Frankfurt, Germany

    Y. Matsushita, A. Dönni, and H. Kitazawa

    • National Institute for Materials Science (NIMS), Tsukuba, Ibaraki 305-0047, Japan

    • *Oksana.Zaharko@psi.ch
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    Issue

    Vol. 78, Iss. 21 — 1 December 2008

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    Images

    • Figure 1
      (Color online) (a) [001] projection of the Na2V3O7 structure. (b) and (c) Arrangement of VO5 square pyramids forming buckled rings (slices A and B) within the unfolded nanotube in the model of Millet et al. (Ref. 1) (b) and in our model (c). (d) Four different families of exchange couplings J1 (gray), J2 (white), J3 (black), and J4 (black dashed). The three sites of vanadium are denoted by V1, V2, V3 in (b), (c). In (d) the notation 11, 12, . . . 34 is used with the first index numbering the site, the second index numbering atoms within the site. Oxygen and sodium atoms are omitted for clarity.Reuse & Permissions
    • Figure 2
      (Color online) Thermal expansion of the lattice parameters a (red/gray filled symbols) and c (blue/gray empty symbols) from x-ray powder diffraction. Inset: the a/c ratio calculated from the SNBL (green/light gray しろまる), SLS (violet/gray ◇) powder patterns, and SNBL (red/gray ◻) single-crystal data.Reuse & Permissions
    • Figure 3
      (Color online) Thermal evolution of the V-V distances calculated from single-crystal x-ray diffraction at 200, 80, and 16 K. Top: first intra-ring distances, bottom: second intra-ring (V11-V22, V21-V31, black), first (V31-V24, V11-V23, red), and second (V11-V12, V31-V33, orange) inter-ring distances.Reuse & Permissions
    • Figure 4
      (Color online) Top: total, nuclear-spin incoherent, and magnetic scattering at 120 K measured on D7 with λi=3.1Å. Inset: the (Q, ω) window accessible during the experiment is shown by the dashed area. Bottom: absolute magnetic scattering at 1.8, 120, and 300 K.Reuse & Permissions
    • Figure 5
      (Color online) Comparison of the magnetic scattering at 2 K measured on D7 and the calculated paramagnetic signal of V4+, both in absolute scale. Calculated low-lying excitations of an isolated nine-member ring and of an isolated dimer are given in arbitrary units.Reuse & Permissions
    • Figure 6
      (Color online) Inelastic neutron scattering (INS) spectra of Na2xV3O7 at 1.5 K and 120 K measured on FOCUS with λi=1.7Å. The intensity has been integrated over the momentum-transfer range 2.1<Q<5.7Å1. Inset: Q dependence at 120 K for 2.6<Q1<3.4Å1 and 4.1<Q2<4.9Å1.Reuse & Permissions
    • Figure 7
      (Color online) Temperature and frequency dependence of real χ and imaginary χ′′ components of ac susceptibility in mK temperature range.Reuse & Permissions
    • Figure 8
      (Color online) Magnetic part of the specific heat divided by temperature Cm/T versus T for different fields. Inset: Cm versus T below 1 K.Reuse & Permissions
    • Figure 9
      (Color online) Temperature and frequency dependence of the normalized remanent magnetization mrem=MtMM0M. Top: the same cooling field of 100 Oe has been used and measurement performed at different temperatures. Inset: Mrem (arb. units) versus T. Bottom: different cooling fields of 100 and 10 Oe have been used and measurement was performed at 40 mK. Inset: A versus Tβ.Reuse & Permissions
    • Figure 10
      (Color online) Temperature dependence of inverse susceptibility obtained from our experiment (symbols) and calculated (solid line) for an isolated nine-member ring with J1=160K and J2=90K. Inset: energy distribution of 512 levels of the ring as a function of the total spin S. Calculations were performed using the ALPS program (Ref. 28).Reuse & Permissions
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