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Signatures for spinons in the quantum spin liquid candidate Ca10Cr7O28

Jonas Sonnenschein, Christian Balz, Ulrich Tutsch, Michael Lang, Hanjo Ryll, Jose A. Rodriguez-Rivera, A. T. M. Nazmul Islam, Bella Lake, and Johannes Reuther
Phys. Rev. B 100, 174428 – Published 25 November 2019

Abstract

We present new experimental low-temperature heat capacity and detailed dynamical spin-structure factor data for the quantum spin-liquid candidate material Ca10Cr7O28. The measured heat capacity shows an almost-perfect linear temperature dependence in the range 0.1KT0.5K, reminiscent of fermionic spinon degrees of freedom. The spin-structure factor exhibits two energy regimes of strong signal which display rather different but solely diffuse scattering features. We theoretically describe these findings by an effective spinon-hopping model which crucially relies on the existence of strong ferromagnetically coupled triangles in the system. Our spinon theory is shown to naturally reproduce the overall weight distribution of the measured spin-structure factor. Particularly, we argue that various different observed characteristic properties of the spin-structure factor and the heat capacity consistently indicate the existence of a spinon Fermi surface. A closer analysis of the heat capacity at the lowest accessible temperatures hints toward the presence of weak f-wave spinon-pairing terms inducing a small partial gap along the Fermi surface (except for discrete nodal Dirac points) and suggesting an overall Z2 quantum spin-liquid scenario for Ca10Cr7O28.

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  • Received 14 June 2019
  • Revised 5 November 2019

DOI:https://doi.org/10.1103/PhysRevB.100.174428

©2019 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Jonas Sonnenschein1,2, Christian Balz3, Ulrich Tutsch4, Michael Lang4, Hanjo Ryll2, Jose A. Rodriguez-Rivera5,6, A. T. M. Nazmul Islam2, Bella Lake2,7, and Johannes Reuther1,2

  • 1Dahlem Center for Complex Quantum Systems and Institut für Theoretische Physik, Freie Universität Berlin, Arnimallee 14, 14195 Berlin, Germany
  • 2Helmholtz-Zentrum für Materialien und Energie, Hahn-Meitner-Platz 1, 14109 Berlin, Germany
  • 3Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA
  • 4Physikalisches Institut, Goethe-Universität Frankfurt, Max-von-Laue-Strasse 1, 60438 Frankfurt, Germany
  • 5NIST Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, Maryland 20899, USA
  • 6Department of Materials Science, University of Maryland, College Park, Maryland 20742, USA
  • 7Institut für Festkörperphysik, Technische Universität Berlin, 10623 Berlin, Germany

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Issue

Vol. 100, Iss. 17 — 1 November 2019

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Images

  • Figure 1
    Figure 1

    (a) Bilayer kagome lattice as realized in Ca10Cr7O28. The differently colored bonds carry the interactions J0,J21,J22,J31, and J32 as indicated in the figure, see also Table 1. (b) Effective decorated honeycomb lattice arising from a projection of the ferromagnetically coupled triangles (green triangles labeled I and J) of the bilayer kagome system into one plane. Bonds are colored and labeled in the same way as in (a), except the antiferromagnetic (blue) bonds, which are not shown for reasons of clarity. Note that sites coupled by the vertical ferromagnetic interlayer couplings (red lines) almost coincide in their position after projection. We have, hence, increased their in-plane distance in this illustration for better visibility. Dark gray (light gray) dots denote sites in the lower (upper) plane. Dashed lines mark the boundaries of the unit cell and numbers label the sites within ferromagnetically coupled triangles. (c) Effective honeycomb lattice with hopping amplitudes ta1,ts2 as they are used in the phenomenological model in Eqs. (5) and (12). In this illustration, each green point corresponds to a ferromagnetic triangle.

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  • Figure 2
    Figure 2

    (a) Measured heat capacity of Ca10Cr7O28 in an extended temperature range. Shown are two different data sets as described in Sec. 2a. The black line indicates the approximate linear behavior at low temperatures. (b) Enlarged view of the low-temperature behavior of the measured heat capacity (relaxation/continuous heating method). Several fits are shown: Linear temperature dependence as obtained for an intact Fermi surface (black line), s-wave-pairing model with a k-independent gap Δs=0.039 meV (gray dashed line), and f-wave-pairing model with the gap function in Eq. (13) using Δf=0.039 meV (blue line). Inset: Heat-capacity data in a double-logarithmic plot. For comparison, the black line shows a T2 temperature dependence. (c) Low-energy spinon band structure for the f-wave-pairing model in Eq. (13) with Δf=0.039 meV. The energy regimes which lead to a linear and quadratic temperature dependence of the heat capacity are indicated.

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  • Figure 3
    Figure 3

    Inelastic neutron-scattering data of Ca10Cr7O28. [(a)–(d)] Constant energy slices as a function of the momentum transfer in the kagome bilayer plane. The black (red) hexagons indicate the boundaries of the first (extended) Brillouin zone. The energy transfer is indicated in each plot. [(e) and (f)] Energy versus momentum slices along two high-symmetry directions within the kagome bilayer plane. The two momentum cuts are illustrated by the gray lines in (d). Note that the color scale is different in each subfigure. The sharp features appearing in red outside the color scale are phonons dispersing from nuclear Bragg peaks. Note that the constant energy slices in (a) and (b) were measured with a final energy of Ef=2.5 meV, which leads to an overall lower intensity compared to the constant energy slices in (c) and (d) measured with Ef=3 meV. For the energy versus momentum slices in (e) and (f) all data were taken with Ef=3 meV. Furthermore, the data in these two plots were collected by integrating the signal over ±0.2 reciprocal lattice units in directions perpendicular to the respective cuts.

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  • Figure 4
    Figure 4

    [(a) and (b)] Weight factors gLL(q) and gLH(q) of the dynamical spin-structure factor S(q,E) as defined in Eqs. (7)–(11) for the spinon-hopping amplitudes given in Eq. (12). Here gLL(q)(gLH(q)) is the total weight factor for all particle-hole excitation processes within the low-energy bands formed by cs (between the low-energy bands formed by cs and the high-energy bands resulting from ca1,ca2). Black (red) dashed lines indicate the boundaries of the first (extended) Brillouin zone. (c) Spinon band structure for the same set of spinon-hopping amplitudes [see Eq. (12)]. Low-energy (high-energy) bands are marked by the corresponding spinon operators cs(ca1 and ca2) they result from. The red line marks the Fermi surface. Note that all bands are doubly degenerate. (d) Illustration of two different particle-hole excitations around the Fermi surface with a given energy E. Process 1 shows an excitation from an occupied state (full black dot) with momentum k and energy ε to an unoccupied state (open dot) with k+q, and ε+E for the minimal momentum transfer q which linearly depends on the energy E. Process 2 is an example for a particle-hole excitation with larger momentum transfer.

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  • Figure 5
    Figure 5

    Calculated spin-structure factor for the effective spinon model in Eq. (5) using the representation of S(q,E) from Eq. (7) and the spinon parameters in Eq. (12). The plots (a)–(d) show the spin-structure factor in momentum space for the same fixed energies E as for the experimental neutron data in Figs. 33. Black (red) dashed lines indicate the boundaries of the first (extended) Brillouin zone. Panels (e) and (f) show S(q,E) as a function of energy along two momentum space directions to compare with Figs. 3 and 3, respectively. The data in (a)–(d) have been convoluted with a Gaussian distribution function to match the experimental resolution while in (e) and (f) the finite-energy resolution and perpendicular q integration have not been taken into account. Note that the magnetic form factor of the Cr5+ ions is not included in these plots.

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  • Figure 6
    Figure 6

    Full inelastic neutron-scattering data for Ca10Cr7O28 at various fixed energy transfers as indicated in each subplot. See text for details.

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