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

Umesh Kumar1,*, Abhishek Nag2,†, Jiemin Li2,3, H. C. Robarts2,4, A. C. Walters2, Mirian García-Fernández2, R. Saint-Martin5, A. Revcolevschi5, Justine Schlappa6 et al.

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

Phys. Rev. B 106, L060406 – Published 18 August, 2022

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

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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