Published November 15, 2021 | Version Published + Supplemental Material + Submitted
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Magnetic order, disorder, and excitations under pressure in the Mott Insulator Sr₂IrO₄

  • 1. ROR icon California Institute of Technology
  • 2. ROR icon Okinawa Institute of Science and Technology
  • 3. ROR icon University of Geneva
  • 4. ROR icon University College London
  • 5. ROR icon Rutherford Appleton Laboratory

Abstract

Protected by the interplay of on-site Coulomb interactions and spin-orbit coupling, Sr₂IrO₄ at high pressure is a rare example of a Mott insulator with a paramagnetic ground state. Here, using optical Raman scattering, we measure both the phonon and magnon evolution in Sr₂IrO₄ under pressure, and identify three different magnetically-ordered phases, culminating in a spin-disordered state beyond 18 GPa. A strong first-order structural phase transition drives the magnetic evolution at ∼10 GPa with reduced structural anisotropy in the IrO₆ cages, leading to increasingly isotropic exchange interactions between the Heisenberg spins and a spin-flip transition to c-axis-aligned antiferromagnetic order. In the disordered phase of Heisenberg J_(eff) = 1/2 pseudospins, the spin excitations are quasi-elastic and continuous to 10 meV, potentially hosting a gapless quantum spin liquid in Sr₂IrO₄.

Additional Information

© 2021 The Author(s). Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI. (Received 7 October 2021; revised 31 October 2021; accepted 2 November 2021; published 19 November 2021) We thank G. Stenning and D. Nye for help with the instruments in the Materials Characterisation Laboratory at the ISIS Neutron and Muon Source. Y.F. acknowledges support from the Okinawa Institute of Science and Technology Graduate University, with subsidy funding from the Cabinet Office, Government of Japan. X.L., D.M.S., and T.F.R. acknowledge support from Air Force Office of Scientific Research Grant No. FA9550-20-1-0263. D.H. acknowledges support from Department of Energy Grant No. DE-SC0010533. F.B. was supported by the Swiss National Science Foundation. A.d.l.T. acknowledges support from the Swiss National Science Foundation through an Early Postdoc Mobility Fellowship (P2GEP2_165044).

Attached Files

Published - PhysRevB.104.L201111.pdf

Submitted - 2110.11588.pdf

Supplemental Material - SI_Sr2IrO4_Raman_10072021.pdf

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Additional details

Additional titles

Alternative title
Magnetic order, disorder, and excitations under pressure in the Mott Insulator Sr2IrO4

Identifiers

Eprint ID
112108
Resolver ID
CaltechAUTHORS:20211130-215730151

Related works

Funding

Okinawa Institute of Science and Technology
Air Force Office of Scientific Research (AFOSR)
FA9550-20-1-0263
Department of Energy (DOE)
DE-SC0010533
Swiss National Science Foundation (SNSF)
P2GEP2_165044

Dates

Created
2021-12-01
Created from EPrint's datestamp field
Updated
2023-06-27
Created from EPrint's last_modified field

Caltech Custom Metadata

Caltech groups
Physics Department