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Magnetic order and dynamics of the charge-ordered antiferromagnet La1.5Sr0.5CoO4

L. M. Helme, A. T. Boothroyd, R. Coldea, D. Prabhakaran, C. D. Frost, D. A. Keen, L. P. Regnault, P. G. Freeman, M. Enderle, and J. Kulda
Phys. Rev. B 80, 134414 – Published 16 October 2009

Abstract

We describe neutron-scattering experiments performed to investigate the magnetic order and dynamics of half-doped La1.5Sr0.5CoO4. This layered perovskite exhibits a near-ideal checkerboard pattern of Co2+/Co3+ charge order at temperatures below 800K. Magnetic correlations are observed at temperatures below 60K but the magnetic order only becomes established at 31 K, a temperature at which a kink is observed in the susceptibility. On warming above 31 K we observed a change in the magnetic correlations which we attribute either to a spin canting or to a change in the proportion of inequivalent magnetic domains. The magnetic excitation spectrum is dominated by an intense band extending above a gap of approximately 3 meV up to a maximum energy of 16 meV. A weaker band exists in the energy range of 20–30 meV. We show that the excitation spectrum is in excellent quantitative agreement with the predictions of a spin-wave theory generalized to include the full magnetic degrees of freedom of high-spin Co2+ ions in an axially distorted crystal field, coupled by Heisenberg exchange interactions. The magnetic order is found to be stabilized by dominant antiferromagnetic Co2+Co2+ interactions acting in a straight line through Co3+. No evidence is found for magnetic scattering from the Co3+ ions, supporting the view that Co3+ is in the S=0 state in this material.

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  • Received 6 July 2009

DOI:https://doi.org/10.1103/PhysRevB.80.134414

©2009 American Physical Society

Authors & Affiliations

L. M. Helme, A. T. Boothroyd*, R. Coldea, and D. Prabhakaran

  • Department of Physics, Oxford University, Oxford OX1 3PU, United Kingdom

C. D. Frost and D. A. Keen

  • ISIS Facility, Rutherford Appleton Laboratory, Chilton, Didcot OX11 0QX, United Kingdom

L. P. Regnault

  • INAC-SPSMS-MDM, CEA—Grenoble, 17 rue des Martyrs, 38054 Grenoble Cedex 9, France

P. G. Freeman, M. Enderle, and J. Kulda

  • Institut Laue-Langevin, Boîte Postale 156, 38042 Grenoble Cedex 9, France

  • *a.boothroyd@physics.ox.ac.uk; http://xray.physics.ox.ac.uk/boothroyd

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Vol. 80, Iss. 13 — 1 October 2009

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Images

  • Figure 1
    Figure 1
    (Color online) (a) Tetragonal unit cell of La2xSrxCoO4. (b) Model for the charge and magnetic orders within the ab plane of La3/2Sr1/2CoO4. The shaded rectangle is the magnetic unit cell. ϕ is the angle of the moments to the a axis, with positive ϕ representing an anticlockwise rotation. The large (yellow) arrow represents the projection of the stacking vector t=(1.5,0.5,0.5) for the spin–charge order.Reuse & Permissions
  • Figure 2
    Figure 2
    (Color online) Part of the Rietveld refinement for tetragonal La1.5Sr0.5CoO4+δ at 60 K. Circles are data measured in the backscattering detector bank (2θ=154.5°) on GEM at ISIS. The solid (red) line shows the calculated profile fit. Tick marks show the positions of allowed reflections, and the solid (blue) line below the data shows the difference between the data and fit. The background fitted in the refinement was subtracted prior to plotting. The fit parameters are given in Table .Reuse & Permissions
  • Figure 3
    Figure 3
    (Color online) Polarized-neutron-diffraction from magnetic and charge orders in La1.5Sr0.5CoO4. (a) Diagram of the (h,k,0) reciprocal-lattice plane showing the in-plane wave vectors of the magnetic order (two twins, unfilled and filled circles marked B and C, respectively) and charge order (crossed circle marked A). The arrows indicate scan directions. (b) l dependence of the charge-order peak at (0.5,0.5,7). (c) and (d) In-plane scans through the magnetic ordering wave vectors in the directions indicated. (e) l dependence of the intensity at the magnetic wave vector marked B. Shaded gray regions contain points contaminated with scattering from aluminum. All scans shown in this figure were made on IN20 with PQ and recorded in both the SF (filled blue circles) and NSF (open red squares) channels. No corrections have been applied for the imperfect neutron polarization. The sample temperature was 2 K.Reuse & Permissions
  • Figure 4
    Figure 4
    (Color online) Temperature dependence of the magnetization of La1.5Sr0.5CoO4. The main frame shows measurements made with the applied field H of strength 100 Oe (μ0H=0.01T) applied parallel to the ab plane. Red filled circles and blue open squares show data from FC and ZFC measurements, respectively. Inset: data up to T=350K showing measurements with both Hab and Hc.Reuse & Permissions
  • Figure 5
    Figure 5
    (Color online) Development of magnetic order in La1.5Sr0.5CoO4. (a) Ratio of the intensities scattered by the projection of the ordered moments along the [110] and [11¯0] directions. Data are from IN20 (filled red circles) and IN22 (filled blue squares). (b) Intensity of the (0.75ϵ,0.75ϵ,1) magnetic Bragg peak. The broken gray line marks the position of the kink in the magnetization (see Fig. 4).Reuse & Permissions
  • Figure 6
    Figure 6
    (Color online) Spin excitation spectrum of La1.5Sr0.5CoO4. (a) Map of the intensity within the (h,k) plane averaged over the energy range of 7–11 meV, measured with a sample temperature of T=10K. The circles centered on the magnetic ordering wave vectors are due to scattering from dispersive magnetic excitations. (b) Energy–Q slice showing the dispersion along the line Y in (a). (c) Energy scan at the magnetic ordering wave vector (0.75ϵ,0.25+ϵ,0) with neutron-polarization analysis to separate the magnetic scattering in the SF channel from the nonmagnetic scattering in the NSF channel. The data were obtained on IN20 at T=2K and reveal an energy gap of 3meV in the magnetic spectrum. (d) Scans along the line X in (a) at temperatures of 10 and 300 K averaged over the energy range of 28–32 meV confirming the existence of magnetic modes at this energy. The data in (a), (b), and (d) were recorded on MAPS, and the intensity is in units of mbsr1meV1f.u.1, where “f.u.” stands for “formula unit” (of La1.5Sr0.5CoO4).Reuse & Permissions
  • Figure 7
    Figure 7
    (Color online) Intensity maps of measured and simulated neutron scattering from La1.5Sr0.5CoO4. The data are from MAPS, and the simulations are obtained from the many-level spin-wave model discussed in the text with Co2+Co2+ exchange interactions J=1.4meV and J1=J2=0 [see Fig. 1b]. (a)–(f) Constant-energy slices averaged over the energy ranges indicated. (g)–(l) Energy–Q slices showing the dispersion along the three symmetry directions indicated. The intensity scale is in units of mbsr1meV1f.u.1.Reuse & Permissions
  • Figure 8
    Figure 8
    (Color online) Dispersion of magnetic excitations in La1.5Sr0.5CoO4. The diagram at the top shows the path in reciprocal space along which the dispersion is plotted. The middle figure shows the measured and calculated dispersion. Symbols are from fits to the experimental data. Circles are from constant-energy cuts, squares and diamonds are from constant wave-vector cuts. The lines are calculated from the many-level spin-orbital model with Co2+Co2+ exchange interactions J=1.4meV and J1=J2=0 [see Fig. 1b]. The lower figure displays the calculated response functions Sαα(Q,ω) for each mode shown in the dispersion plot. The labels on the curves give the αα components for the case in which the ordered moments point along x.Reuse & Permissions
  • Figure 9
    Figure 9
    Single-ion energy levels of the F4 term of Co2+ in La1.5Sr0.5CoO4, showing how the term splits when successively smaller interactions are added. The splitting caused by the axially distorted crystal field is obtained with coefficients B20=13meV, B40=1.4meV, and B44=8meV for the Stevens operator equivalents O20, O40, and O44. These values are approximately twice those calculated from the point-charge model. The right-most scheme includes spin-orbit coupling and shows the splitting of the lowest orbital quasitriplet on an expanded vertical scale. The spin-orbit coupling parameter is λ=18.7meV.Reuse & Permissions
  • Figure 10
    Figure 10
    (Color online) Magnetic dispersion parallel to the (h,0) direction in La1.5Sr0.5CoO4. The symbols are points determined from energy cuts at constant wave vector through the MAPS data. Full and broken lines are in-plane and out-of-plane modes of the effective spin-12 ground-state doublet calculated from Eq. (2) by linear spin-wave theory with the following exchange parameters: (i) SJ=3.68meV and J1=J2=J/2; (ii) SJ=3.23meV and SJ1=SJ2=0.15meV; and (iii) SJ=2.85meV and J1=J2=J/2. The parameters in (ii) have been adjusted to give the best fit to the data. In each case the exchange-anisotropy parameters were ε=0.03 and δ=0.65.Reuse & Permissions
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