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  • Letter
  • Open Access

Magnetic order, disorder, and excitations under pressure in the Mott insulator Sr2IrO4

Xiang Li1,2, S. E. Cooper2, A. Krishnadas2, A. de la Torre1,3, R. S. Perry4,5, F. Baumberger3, D. M. Silevitch1, D. Hsieh1, T. F. Rosenbaum1,* et al.

Yejun Feng1,2,†

  • 1Division of Physics, Mathematics, and Astronomy, California Institute of Technology, Pasadena, California 91125, USA
  • 2Okinawa Institute of Science and Technology Graduate University, Onna, Okinawa 904-0495, Japan
  • 3Department of Quantum Matter Physics, University of Geneva, 1211 Geneva 4, Switzerland
  • 4London Centre for Nanotechnology and Department of Physics and Astronomy, University College London, London WC1E 6BT, United Kingdom
  • 5ISIS Facility, Rutherford Appleton Laboratory, Didcot OX11 0QX, United Kingdom

  • *Corresponding author: tfr@caltech.edu
  • †Corresponding author: yejun@oist.jp

Phys. Rev. B 104, L201111 – Published 19 November, 2021

DOI: https://doi.org/10.1103/PhysRevB.104.L201111

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 Jeff=1/2 pseudospins, the spin excitations are quasielastic and continuous to 10 meV, potentially hosting a gapless quantum spin liquid in Sr2IrO4.

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