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  • Letter

Unraveling higher-order contributions to spin excitations probed using resonant inelastic x-ray scattering

Umesh Kumar, Abhishek Nag, Jiemin Li, H. C. Robarts, A. C. Walters, Mirian García-Fernández, R. Saint-Martin, A. Revcolevschi, Justine Schlappa, Thorsten Schmitt, Steven Johnston, and Ke-Jin Zhou
Phys. Rev. B 106, L060406 – Published 18 August 2022
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Abstract

Resonant inelastic x-ray scattering (RIXS) is an evolving tool for investigating the spin dynamics of strongly correlated materials, which complements inelastic neutron scattering. In isotropic spin-12 Heisenberg antiferromagnetic (HAFM) spin chains, both techniques have observed non-spin-conserving (NSC) excitations confined to the two-spinon phase space. However, a recent O K-edge RIXS study of the one-dimensional HAFM Sr2CuO3 observed spin-conserving (SC) four-spinon excitations outside the two-spinon phase space. Here, we demonstrate that analogous four-spinon excitations can also be accessed at the Cu L3 edge in the related material SrCuO2. Through detailed modeling, we establish that these excitations appear in both the SC and NSC channels of the Cu L3 edge, and are only captured by higher-order terms in the ultrashort core-hole lifetime expansion. Since these terms encode information about spin-spin correlations extending beyond nearest neighbors, our results offer different possibilities for studying nonlocal spin correlations in quantum magnets.

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  • Received 24 September 2021
  • Revised 17 January 2022
  • Accepted 3 August 2022

DOI:https://doi.org/10.1103/PhysRevB.106.L060406

©2022 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Umesh Kumar1,*, Abhishek Nag2,†, Jiemin Li2,3, H. C. Robarts2,4, A. C. Walters2, Mirian García-Fernández2, R. Saint-Martin5, A. Revcolevschi5, Justine Schlappa6, Thorsten Schmitt7, Steven Johnston8,9, and Ke-Jin Zhou2,‡

  • 1Theoretical Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA
  • 2Diamond Light Source, Harwell Campus, Didcot OX11 0DE, United Kingdom
  • 3Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China
  • 4H. H. Wills Physics Laboratory, University of Bristol, Bristol BS8 1TL, United Kingdom
  • 5Institut de Chimie Moléculaire et des Matériaux d'Orsay, Université Paris-Saclay, UMR 8182, 91405 Orsay, France
  • 6European X-Ray Free-Electron Laser Facility GmbH, Holzkoppel 4, 22869 Schenefeld, Germany
  • 7Photon Science Division, Paul Scherrer Institut, 5232 Villigen PSI, Switzerland
  • 8Department of Physics and Astronomy, The University of Tennessee, Knoxville, Tennessee 37996, USA
  • 9Institute for Advanced Materials and Manufacturing, University of Tennessee, Knoxville, Tennessee 37996, USA

  • *umesh.kumar@rutgers.edu
  • abhishek.nag@diamond.ac.uk
  • kejin.zhou@diamond.ac.uk

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Issue

Vol. 106, Iss. 6 — 1 August 2022

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Images

  • Figure 1
    Figure 1

    (a) A schematic diagram of the RIXS scattering geometry for SrCuO2. (b) and (c) show the low-energy Cu L3- and O K-edge RIXS spectra, respectively, measured at q=0.175. (d) and (e) show the corresponding data at q=0. Also shown in (d) is the RIXS spectrum multiplied by a factor of five and vertically shifted. At q=0, the energy of the two-spinon excitations and their spectral weight are zero. For q=0.175, the two-spinons are approximated by the Müller ansatz [44]. The vertical dashed line indicates the upper boundary of the four-spinon continuum [45]. In all cases, additional spectral weight (marked by arrows) is observed outside the two-spinon phase space but inside the four-spinon phase space.

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  • Figure 2
    Figure 2

    (a) O K-edge and (b) Cu L3-edge RIXS intensity maps for momentum transfer along the chain. The brown color represents the maximum spectral weight in the color scale. The two-spinon continuum boundaries are shown by blue dashed lines. Horizontal dashed green lines mark the higher-energy limit of the phonon excitations. The RIXS spectra shown in Figs. 1 correspond to the vertical black dashed lines. Model intensity maps for spin excitations at the (c) O K edge and (d) Cu L3 edge computed using the Kramers-Heisenberg formalism.

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  • Figure 3
    Figure 3

    The calculated Cu L3-edge RIXS spectra in the (a) NSC and (b) SC channels, computed using the Kramers-Heisenberg formalism. The brown color represents the maximum spectral weight in the color scale. (c) The normalized intensity profiles of the two spin channels obtained by integrating the region marked by the red dashed lines in (b) and (c). (d) The integrated intensity profile for the same region obtained from the Cu L3-edge RIXS experiment on SrCuO2. The continuous line is a weighted sum of the NSC and SC channel profiles shown in (c) and a linear background to match the experimental profile (see text).

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  • Figure 4
    Figure 4

    The generalized dynamical structure factors S(N)SCk(q,ω) appearing in higher-order terms of the UCL expansion. (a) and (b) show the intensity maps of the first-order (k=1) terms in the NSC and SC channels, respectively. (c) and (d) show the intensity maps of the second-order (k=2) terms in the NSC and SC channels, respectively. The brown color represents the maximum spectral weight in the color scale.

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