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Title: Structural, electronic, and magnetic properties of nearly ideal Jeff = 1/2 iridium halides

Abstract

Heavy transition metal magnets with J(eff) = 1/2 electronic ground states have attracted recent interest due to their penchant for hosting new classes of quantum spin liquids and superconductors. Unfortunately, model systems with ideal J(eff) = 1/2 states are scarce due to the importance of noncubic local distortions in most candidate materials. In this work, we identify a family of iridium halide systems [i.e., K2IrCl6, K2IrBr6, (NH4)(2)IrCl6, and Na2IrCl6.6(H2O)] with Ir-4(+) electronic ground states exhibiting extremely small deviations from the ideal J(eff) =1 limit. We also find ordered magnetic ground states for the three anhydrous systems, with single-crystal neutron diffraction on K2IrBr6 revealing type-I antiferromagnetism. This spin configuration is consistent with expectations for significant Kitaev exchange in a face-centered-cubic magnet. This work establishes that incorporating isolated IrX6 octahedra in materials, where X is a halogen ion with a low electronegativity, is an effective design principle for realizing unprecedented proximity to the pure J(eff) = state. At the same time, we highlight undeniable deviations from this ideal state, even in clean materials with ideal IrX6 octahedra as inferred from the global cubic crystal structures.

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [3];  [4];  [5]; ORCiD logo [6]; ORCiD logo [6]; ORCiD logo [3];  [7]; ORCiD logo [6]; ORCiD logo [2]
  1. Univ. of Illinois at Urbana-Champaign, IL (United States); Univ. of British Columbia, Vancouver, BC (Canada)
  2. Univ. of Illinois at Urbana-Champaign, IL (United States)
  3. Univ. of Tennessee, Knoxville, TN (United States)
  4. Cornell Univ., Ithaca, NY (United States). Cornell High Energy Synchrotron Source (CHESS)
  5. Argonne National Lab. (ANL), Lemont, IL (United States). Advanced Photon Source (APS)
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  7. McMaster Univ., Hamilton, ON (Canada)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1755299
Alternate Identifier(s):
OSTI ID: 1787598
Grant/Contract Number:  
AC05-00OR22725; AC02-06CH11357; DMR-1332208; DMR-1829070; DMR-1455264; DMR-2003117
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 4; Journal Issue: 12; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Magnetic order; magnetic phase transitions; magnetism; spin-orbit coupling; structural properties

Citation Formats

Reig-i-Plessis, D., Johnson, T. A., Lu, K., Chen, Q., Ruff, J. C., Upton, M. H., Williams, T. J., Calder, S., Zhou, H. D., Clancy, J. P., Aczel, A. A., and MacDougall, G. J.. Structural, electronic, and magnetic properties of nearly ideal Jeff = 1/2 iridium halides. United States: N. p., 2020. Web. https://doi.org/10.1103/physrevmaterials.4.124407.
Reig-i-Plessis, D., Johnson, T. A., Lu, K., Chen, Q., Ruff, J. C., Upton, M. H., Williams, T. J., Calder, S., Zhou, H. D., Clancy, J. P., Aczel, A. A., & MacDougall, G. J.. Structural, electronic, and magnetic properties of nearly ideal Jeff = 1/2 iridium halides. United States. https://doi.org/10.1103/physrevmaterials.4.124407
Reig-i-Plessis, D., Johnson, T. A., Lu, K., Chen, Q., Ruff, J. C., Upton, M. H., Williams, T. J., Calder, S., Zhou, H. D., Clancy, J. P., Aczel, A. A., and MacDougall, G. J.. Thu . "Structural, electronic, and magnetic properties of nearly ideal Jeff = 1/2 iridium halides". United States. https://doi.org/10.1103/physrevmaterials.4.124407.
@article{osti_1755299,
title = {Structural, electronic, and magnetic properties of nearly ideal Jeff = 1/2 iridium halides},
author = {Reig-i-Plessis, D. and Johnson, T. A. and Lu, K. and Chen, Q. and Ruff, J. C. and Upton, M. H. and Williams, T. J. and Calder, S. and Zhou, H. D. and Clancy, J. P. and Aczel, A. A. and MacDougall, G. J.},
abstractNote = {Heavy transition metal magnets with J(eff) = 1/2 electronic ground states have attracted recent interest due to their penchant for hosting new classes of quantum spin liquids and superconductors. Unfortunately, model systems with ideal J(eff) = 1/2 states are scarce due to the importance of noncubic local distortions in most candidate materials. In this work, we identify a family of iridium halide systems [i.e., K2IrCl6, K2IrBr6, (NH4)(2)IrCl6, and Na2IrCl6.6(H2O)] with Ir-4(+) electronic ground states exhibiting extremely small deviations from the ideal J(eff) =1 limit. We also find ordered magnetic ground states for the three anhydrous systems, with single-crystal neutron diffraction on K2IrBr6 revealing type-I antiferromagnetism. This spin configuration is consistent with expectations for significant Kitaev exchange in a face-centered-cubic magnet. This work establishes that incorporating isolated IrX6 octahedra in materials, where X is a halogen ion with a low electronegativity, is an effective design principle for realizing unprecedented proximity to the pure J(eff) = state. At the same time, we highlight undeniable deviations from this ideal state, even in clean materials with ideal IrX6 octahedra as inferred from the global cubic crystal structures.},
doi = {10.1103/physrevmaterials.4.124407},
journal = {Physical Review Materials},
number = 12,
volume = 4,
place = {United States},
year = {2020},
month = {12}
}

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