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Title: Pressure-induced structural dimerization in the hyperhoneycomb iridate β Li 2 IrO 3 at low temperatures

Abstract

A pressure-induced collapse of magnetic ordering in β-Li 2IrO 3 at P m similar to 1.5-2 GPa has previously been interpreted as evidence for potential emergence of spin liquid states in this hyperhoneycomb iridate, raising prospects for experimental realizations of the Kitaev model. Based on structural data obtained at room temperature, this magnetic transition is believed to originate in small lattice perturbations that preserve crystal symmetry, and related changes in bond-directional anisotropic exchange interactions. In this work, we report on the evolution of the crystal structure of β-Li 2IrO 3 under pressure at low temperatures (T ≤ 50 K) and show that the suppression of magnetism coincides with a change in lattice symmetry involving Ir-Ir dimerization. The critical pressure for dimerization shifts from 4.4(2) GPa at room temperature to similar to 1.5-2 GPa below 50 K. While a direct Fddd → C-2/c transition is observed at room temperature, the low temperature transitions involve new as well as coexisting dimerized phases. Additional investigation of the Ir (L 3/L 2) isotropic branching ratio in x-ray absorption spectra indicates that the previously reported departure of the electronic ground state from a J eff = 1/2 state is closely related to the onset ofmore » dimerized phases. In essence, our results suggest that the predominant mechanism driving the collapse of magnetism in β-Li 2IrO 3 is the pressure-induced formation of Ir 2 dimers in the hyperhoneycomb network. The results further confirm the instability of the J eff = 1/2 moments and related noncollinear spiral magnetic ordering against formation of dimers in the low-temperature phase of compressed β-Li 2IrO 3.« less

Authors:
ORCiD logo [1];  [2];  [3];  [1];  [1];  [4];  [2];  [5];  [6];  [1];  [7];  [7];  [3]
  1. Univ. College London, Bloomsbury (United Kingdom)
  2. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Univ. of Illinois, Chicago, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Ehime Univ., Matsuyama (Japan); Tokyo Institute of Technology (Japan)
  6. European Synchrotron Radiation Facility (ESRF), Grenoble (France)
  7. Max Planck Inst. for Solid State Research, Stuttgart (Germany); Univ. of Tokyo (Japan)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1574949
Alternate Identifier(s):
OSTI ID: 1558155
Grant/Contract Number:  
AC02-06CH11357; AC-02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 100; Journal Issue: 6; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Veiga, L. S. I., Glazyrin, K., Fabbris, G., Dashwood, C. D., Vale, J. G., Park, H., Etter, M., Irifune, T., Pascarelli, S., McMorrow, D. F., Takayama, T., Takagi, H., and Haskel, D. Pressure-induced structural dimerization in the hyperhoneycomb iridate β−Li2IrO3 at low temperatures. United States: N. p., 2019. Web. doi:10.1103/PhysRevB.100.064104.
Veiga, L. S. I., Glazyrin, K., Fabbris, G., Dashwood, C. D., Vale, J. G., Park, H., Etter, M., Irifune, T., Pascarelli, S., McMorrow, D. F., Takayama, T., Takagi, H., & Haskel, D. Pressure-induced structural dimerization in the hyperhoneycomb iridate β−Li2IrO3 at low temperatures. United States. doi:10.1103/PhysRevB.100.064104.
Veiga, L. S. I., Glazyrin, K., Fabbris, G., Dashwood, C. D., Vale, J. G., Park, H., Etter, M., Irifune, T., Pascarelli, S., McMorrow, D. F., Takayama, T., Takagi, H., and Haskel, D. Wed . "Pressure-induced structural dimerization in the hyperhoneycomb iridate β−Li2IrO3 at low temperatures". United States. doi:10.1103/PhysRevB.100.064104.
@article{osti_1574949,
title = {Pressure-induced structural dimerization in the hyperhoneycomb iridate β−Li2IrO3 at low temperatures},
author = {Veiga, L. S. I. and Glazyrin, K. and Fabbris, G. and Dashwood, C. D. and Vale, J. G. and Park, H. and Etter, M. and Irifune, T. and Pascarelli, S. and McMorrow, D. F. and Takayama, T. and Takagi, H. and Haskel, D.},
abstractNote = {A pressure-induced collapse of magnetic ordering in β-Li2IrO3 at Pm similar to 1.5-2 GPa has previously been interpreted as evidence for potential emergence of spin liquid states in this hyperhoneycomb iridate, raising prospects for experimental realizations of the Kitaev model. Based on structural data obtained at room temperature, this magnetic transition is believed to originate in small lattice perturbations that preserve crystal symmetry, and related changes in bond-directional anisotropic exchange interactions. In this work, we report on the evolution of the crystal structure of β-Li2IrO3 under pressure at low temperatures (T ≤ 50 K) and show that the suppression of magnetism coincides with a change in lattice symmetry involving Ir-Ir dimerization. The critical pressure for dimerization shifts from 4.4(2) GPa at room temperature to similar to 1.5-2 GPa below 50 K. While a direct Fddd → C-2/c transition is observed at room temperature, the low temperature transitions involve new as well as coexisting dimerized phases. Additional investigation of the Ir (L3/L2) isotropic branching ratio in x-ray absorption spectra indicates that the previously reported departure of the electronic ground state from a Jeff = 1/2 state is closely related to the onset of dimerized phases. In essence, our results suggest that the predominant mechanism driving the collapse of magnetism in β-Li2IrO3 is the pressure-induced formation of Ir2 dimers in the hyperhoneycomb network. The results further confirm the instability of the Jeff = 1/2 moments and related noncollinear spiral magnetic ordering against formation of dimers in the low-temperature phase of compressed β-Li2IrO3.},
doi = {10.1103/PhysRevB.100.064104},
journal = {Physical Review B},
number = 6,
volume = 100,
place = {United States},
year = {2019},
month = {8}
}

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