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Title: Decoupling of the antiferromagnetic and insulating states in Tb-doped Sr2IrO4

Abstract

Sr2IrO4 is a spin-orbit coupled insulator with an antiferromagnetic (AFM) transition at TN=240 K. We report results of a comprehensive study of single-crystal Sr2Ir1-xTbxO4 (0 x 0.03). This study found that mere 3% (x=0.03) tetravalent Tb4+(4f7) substituting for Ir4+ (rather than Sr2+) completely suppresses the long-range AFM transition but stabilizes the insulating state, leading to a phase diagram featuring a decoupling of magnetic interactions and charge gap. The insulating state at x=0.03 is characterized by an unusually large specific heat at low temperatures and an incommensurate magnetic state having a magnetic peak at (0.95, 0, 0) in the neutron diffraction. It is apparent that Tb doping effectively changes the relative strength of the SOI and the tetragonal CEF and enhances the Hund's rule coupling that competes with the SOI, and destabilizes the AFM state. However, the disappearance of the AFM accompanies no metallic state chiefly because an energy level mismatch for the Ir and Tb sites weakens charge carrier hopping and renders a persistent insulating state. This work highlights an unconventional correlation between the AFM and insulating states in which the magnetic transition plays no critical role in formation of charge gap in the iridate.

Authors:
 [1];  [2];  [3];  [2];  [2];  [4];  [5];  [4];  [6];  [7];  [2];  [2]
  1. Univ. of Kentucky, Lexington, KY (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Renmin Univ. of China, Beijing (China)
  2. Univ. of Kentucky, Lexington, KY (United States)
  3. Univ. of Kentucky, Lexington, KY (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  6. Florida State Univ., Tallahassee, FL (United States)
  7. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). High Flux Isotope Reactor (HFIR); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1248025
Alternate Identifier(s):
OSTI ID: 1228425; OSTI ID: 1324063
Grant/Contract Number:  
AC02-06CH11357; FG02-98ER45707; AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review. B, Condensed Matter and Materials Physics
Additional Journal Information:
Journal Volume: 92; Journal Issue: 21; Journal ID: ISSN 1098-0121
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE

Citation Formats

Wang, J. C., Aswartham, S., Ye, Feng, Terzic, J., Zheng, H., Haskel, Daniel, Chikara, Shalinee, Choi, Yong, Schlottmann, P., Custelcean, Radu, Yuan, S. J., and Cao, G. Decoupling of the antiferromagnetic and insulating states in Tb-doped Sr2IrO4. United States: N. p., 2015. Web. doi:10.1103/PhysRevB.92.214411.
Wang, J. C., Aswartham, S., Ye, Feng, Terzic, J., Zheng, H., Haskel, Daniel, Chikara, Shalinee, Choi, Yong, Schlottmann, P., Custelcean, Radu, Yuan, S. J., & Cao, G. Decoupling of the antiferromagnetic and insulating states in Tb-doped Sr2IrO4. United States. https://doi.org/10.1103/PhysRevB.92.214411
Wang, J. C., Aswartham, S., Ye, Feng, Terzic, J., Zheng, H., Haskel, Daniel, Chikara, Shalinee, Choi, Yong, Schlottmann, P., Custelcean, Radu, Yuan, S. J., and Cao, G. Tue . "Decoupling of the antiferromagnetic and insulating states in Tb-doped Sr2IrO4". United States. https://doi.org/10.1103/PhysRevB.92.214411. https://www.osti.gov/servlets/purl/1248025.
@article{osti_1248025,
title = {Decoupling of the antiferromagnetic and insulating states in Tb-doped Sr2IrO4},
author = {Wang, J. C. and Aswartham, S. and Ye, Feng and Terzic, J. and Zheng, H. and Haskel, Daniel and Chikara, Shalinee and Choi, Yong and Schlottmann, P. and Custelcean, Radu and Yuan, S. J. and Cao, G.},
abstractNote = {Sr2IrO4 is a spin-orbit coupled insulator with an antiferromagnetic (AFM) transition at TN=240 K. We report results of a comprehensive study of single-crystal Sr2Ir1-xTbxO4 (0 x 0.03). This study found that mere 3% (x=0.03) tetravalent Tb4+(4f7) substituting for Ir4+ (rather than Sr2+) completely suppresses the long-range AFM transition but stabilizes the insulating state, leading to a phase diagram featuring a decoupling of magnetic interactions and charge gap. The insulating state at x=0.03 is characterized by an unusually large specific heat at low temperatures and an incommensurate magnetic state having a magnetic peak at (0.95, 0, 0) in the neutron diffraction. It is apparent that Tb doping effectively changes the relative strength of the SOI and the tetragonal CEF and enhances the Hund's rule coupling that competes with the SOI, and destabilizes the AFM state. However, the disappearance of the AFM accompanies no metallic state chiefly because an energy level mismatch for the Ir and Tb sites weakens charge carrier hopping and renders a persistent insulating state. This work highlights an unconventional correlation between the AFM and insulating states in which the magnetic transition plays no critical role in formation of charge gap in the iridate.},
doi = {10.1103/PhysRevB.92.214411},
journal = {Physical Review. B, Condensed Matter and Materials Physics},
number = 21,
volume = 92,
place = {United States},
year = {Tue Dec 08 00:00:00 EST 2015},
month = {Tue Dec 08 00:00:00 EST 2015}
}

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Works referencing / citing this record:

The challenge of spin–orbit-tuned ground states in iridates: a key issues review
journal, February 2018


The J eff = 1/2 Antiferromagnet Sr 2 IrO 4 : A Golden Avenue toward New Physics and Functions
journal, October 2019


Single-phased chromaticity-tunable phosphor of Sr 4 Al 14 O 25 : Eu 2+/3+ co-doped with Tb 3+ for white-light-emitting diodes
journal, September 2019


Synthesis and physical properties of the new iridium oxyfluoride S r 2 Ir ( O , F ) 6 δ using a topochemical reaction method
journal, January 2020