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Collinear antiferromagnetic order in URu2Si2xPx revealed by neutron diffraction

M. C. Rahn, A. Gallagher, F. Orlandi, D. D. Khalyavin, C. Hoffmann, P. Manuel, R. Baumbach, and M. Janoschek
Phys. Rev. B 103, 214403 – Published 1 June 2021
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Abstract

The hidden order phase in URu2Si2 is highly sensitive to electronic doping. A special interest in silicon-to-phosphorus substitution is due to the fact that it may allow one, in part, to isolate the effects of tuning the chemical potential from the complexity of the correlated f and d electronic states. We investigate the new antiferromagnetic phase that is induced in URu2Si2xPx at x0.27. Time-of-flight neutron diffraction of a single crystal (x=0.28) reveals c-axis collinear qm=(12,12,12) magnetic order with localized magnetic moments (2.12.6μB). This points to an unexpected analogy between the (Si,P) and (Ru,Rh) substitution series. Through further comparisons with other tuning studies of URu2Si2, we are able to delineate the mechanisms by which silicon-to-phosphorus substitution affects the system. In particular, both the localization of itinerant 5f electrons as well as the choice of qm appear to be consequences of the increase in chemical potential. Further, enhanced exchange interactions are induced by chemical pressure and lead to magnetic order, in which an increase in interlayer spacing may play a special role.

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  • Received 3 February 2021
  • Revised 16 May 2021
  • Accepted 17 May 2021

DOI:https://doi.org/10.1103/PhysRevB.103.214403

©2021 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

M. C. Rahn1,2,*, A. Gallagher3, F. Orlandi4, D. D. Khalyavin4, C. Hoffmann5, P. Manuel4, R. Baumbach3, and M. Janoschek1,6,7,†

  • 1Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA
  • 2Institute for Solid State and Materials Physics, Technical University of Dresden, 01062 Dresden, Germany
  • 3National High Magnetic Field Laboratory, Florida State University, Tallahassee, Florida 32310, USA
  • 4ISIS Facility, STFC, Rutherford Appleton Laboratory, Chilton, Didcot, Oxfordshire OX11 0QX, United Kingdom
  • 5Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, USA
  • 6Laboratory for Neutron and Muon Instrumentation, Paul Scherrer Institute, CH-5232 Villigen, Switzerland
  • 7Physik-Institut, Universität Zürich, CH-8057 Zürich, Switzerland

  • *marein.rahn@tu-dresden.de
  • marc.janoschek@psi.ch

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Vol. 103, Iss. 21 — 1 June 2021

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Images

  • Figure 1
    Figure 1

    Simplified phase diagram of URu2Si2xPx, adapted from Gallagher et al. [59]. Few percents of phosphorus substitution suppress the hidden order (HO) and, with it, superconductivity (SC). The arrow marks the composition of the long-range antiferromagnetically (AFM) ordered sample investigated in this study.

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  • Figure 2
    Figure 2

    (a) Overview of Bragg peaks observed at WISH, at 2 K. The upper (lower) panel shows the raw neutron counts detected on the left (right) detector bank, on an arbitrary logarithmic scale. The (101)–(01¯1) plane of reciprocal space is indicated by a white dashed line. The (1,1,1) direction, which features the only observed magnetic Bragg peak, is seen below this plane, at a scattering angle of around 30. (b) Perspective view of this data, illustrating the layout of the instrument. (c) Schematic view of the (101)–(01¯1) plane of reciprocal space (Note that the magnetic peak at qm is observed below this plane). The accessible range of momentum transfers is delineated by a broad gray line and peaks seen in (a) are labeled in analogy. The dotted line indicates the momentum transfer at which the magnetic form factor of uranium has decreased by 1/e ( 5.5 Å1).

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  • Figure 3
    Figure 3

    Magnetic susceptibility of the URu2Si2xPx (x=0.28) crystal investigated by neutron diffraction, in a field of 0.5 T applied either parallel or perpendicular to the c axis. The right panel shows a detailed view of the Hc data. As in the parent compound, the characteristics are dominated by the onset of Kondo screening around Tcoh80 K, as well as a strong c-axis single-ion anisotropy.

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  • Figure 4
    Figure 4

    Comparison of Bragg intensities calculated for URu2Si2xPx (x=0.28) with those measured at WISH at 2 K. The overall scale factor was inferred from a refinement of nuclear intensities (red). The magnitude of the ordered magnetic moment was then fitted separately to reproduce the intensities of magnetic reflections (green). Numerical values of these fits are given in the Supplemental Material [68].

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  • Figure 5
    Figure 5

    Temperature dependence of the ordered magnetic moment in URu2Si2xPx (x=0.28), with an ordering temperature of TN=32.6(7) K and critical exponent β=0.31(4). The inset illustrates the emergence of a magnetic Bragg reflection at momentum transfer Q=qm=(12,12,12).

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  • Figure 6
    Figure 6

    c-axis collinear qm=(12,12,12) magnetic structure of URu2Si2xPx (x=0.28), described by the Shubnikov group Ic41/acd (No. 142.570). For clarity, only uranium ions are shown and opposite spins are drawn in different colors.

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  • Figure 7
    Figure 7

    Changes of the lattice parameters a (top) and c (bottom) in the (Ru,Rh) and (Si,P) substitution series. The data are adapted from studies by Burlet et al. [45] and Gallagher et al. [59]. In the lower panel, the critical compositions at which local moment qm=(12,12,12) magnetic order emerges in either series are marked by arrows.

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  • Figure 8
    Figure 8

    Pressure dependence of the heavy-fermion coherence scale Tcoh, inferred from a broad maximum in magnetic susceptibility χ(T) curves (cf. Fig. 3). Data for chemical pressure in the present doping series, adapted from Ref. [59], is compared to measurements of the parent compound under applied pressure, reported by Pfleiderer et al. [81]. The arrows and shaded margins indicate the regimes where long-range magnetic order is induced by hydrostatic (red) and chemical (black) pressure.

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