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

Kumar, Umesh; Nag, Abhishek; Li, Jiemin; Robarts, H. C.; Walters, A. C.; García-Fernández, Mirian; Saint-Martin, Romuald; Revcolevschi, A.; Schlappa, Justine; Schmitt, Thorsten; Johnston, Steven; Zhou, Ke-Jin

doi:10.1103/physrevb.106.l060406

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

Journal Article · Thu Aug 18 00:00:00 EDT 2022 · Physical Review. B

DOI:https://doi.org/10.1103/physrevb.106.l060406· OSTI ID:1998115

^[1]; Nag, Abhishek ^[2]; Li, Jiemin ^[3]; Robarts, H. C. ^[4]; ^[2]; ^[2]; ^[5]; Revcolevschi, A. ^[5]; Schlappa, Justine ^[6]; Schmitt, Thorsten ^[7]; Johnston, Steven ^[8]; ^[2]

Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Science and Technology Facilities Council (STFC), Oxford (United Kingdom). Diamond Light Source, Ltd.
Science and Technology Facilities Council (STFC), Oxford (United Kingdom). Diamond Light Source, Ltd.; Chinese Academy of Sciences (CAS), Beijing (China). Beijing National Laboratory for Condensed Matter Physics and Institute of Physics
Science and Technology Facilities Council (STFC), Oxford (United Kingdom). Diamond Light Source, Ltd.; Univ. of Bristol (United Kingdom)
Univ. Paris-Saclay, Orsay (France)
European XFEL, Schenefeld (Germany)
Paul Scherrer Inst. (PSI), Villigen (Switzerland)
Univ. of Tennessee, Knoxville, TN (United States)

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-$$\frac{1}{2}$$ 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 Sr₂ CuO₃ 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. Finally, 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.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: National Science Foundation (NSF); Swiss National Science Foundation (SNSF); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1998115

Report Number(s):: LA-UR--21-29415

Journal Information:: Physical Review. B, Journal Name: Physical Review. B Journal Issue: 6 Vol. 106; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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