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:
-
- Univ. of Kentucky, Lexington, KY (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Renmin Univ. of China, Beijing (China)
- Univ. of Kentucky, Lexington, KY (United States)
- Univ. of Kentucky, Lexington, KY (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Florida State Univ., Tallahassee, FL (United States)
- 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}
}
Web of Science
Works referenced in this record:
Atomically resolved spectroscopic study of Sr2IrO4: Experiment and theory
journal, October 2013
- Li, Qing; Cao, Guixin; Okamoto, Satoshi
- Scientific Reports, Vol. 3, Issue 1
Coulomb gap and low temperature conductivity of disordered systems
journal, February 1975
- Efros, A. L.; Shklovskii, B. I.
- Journal of Physics C: Solid State Physics, Vol. 8, Issue 4
Sr2RhO4 and Sr2IrO4: Structural and magnetic studies of 4d and 5d transition metal analogs of La2CuO4
journal, December 1994
- Subramanian, M. A.; Crawford, M. K.; Harlow, R. L.
- Physica C: Superconductivity, Vol. 235-240
Transport and thermal properties of weakly ferromagnetic Sr 2 IrO 4
journal, August 2006
- Kini, N. S.; Strydom, A. M.; Jeevan, H. S.
- Journal of Physics: Condensed Matter, Vol. 18, Issue 35
Phase-Sensitive Observation of a Spin-Orbital Mott State in Sr2IrO4
journal, March 2009
- Kim, B. J.; Ohsumi, H.; Komesu, T.
- Science, Vol. 323, Issue 5919
Fermi arcs in a doped pseudospin-1/2 Heisenberg antiferromagnet
journal, June 2014
- Kim, Y. K.; Krupin, O.; Denlinger, J. D.
- Science, Vol. 345, Issue 6193
Persistent non-metallic behavior in Sr 2 IrO 4 and Sr 3 Ir 2 O 7 at high pressures
journal, June 2014
- Zocco, D. A.; Hamlin, J. J.; White, B. D.
- Journal of Physics: Condensed Matter, Vol. 26, Issue 25
Weak ferromagnetism, metal-to-nonmetal transition, and negative differential resistivity in single-crystal
journal, May 1998
- Cao, G.; Bolivar, J.; McCall, S.
- Physical Review B, Vol. 57, Issue 18
Novel Mott State Induced by Relativistic Spin-Orbit Coupling in
journal, August 2008
- Kim, B. J.; Jin, Hosub; Moon, S. J.
- Physical Review Letters, Vol. 101, Issue 7
Dimensionality-Controlled Insulator-Metal Transition and Correlated Metallic State in Transition Metal Oxides ( , 2, and )
journal, November 2008
- Moon, S. J.; Jin, H.; Kim, K. W.
- Physical Review Letters, Vol. 101, Issue 22
Magnetic Excitation Spectra of Probed by Resonant Inelastic X-Ray Scattering: Establishing Links to Cuprate Superconductors
journal, April 2012
- Kim, Jungho; Casa, D.; Upton, M. H.
- Physical Review Letters, Vol. 108, Issue 17
Two-Dimensional Heisenberg Behavior of Isospins in the Paramagnetic State of the Spin-Orbital Mott Insulator
journal, June 2012
- Fujiyama, S.; Ohsumi, H.; Komesu, T.
- Physical Review Letters, Vol. 108, Issue 24
Dimensionality-controlled Mott transition and correlation effects in single-layer and bilayer perovskite iridates
journal, June 2013
- Wang, Q.; Cao, Y.; Waugh, J. A.
- Physical Review B, Vol. 87, Issue 24
Local density of states study of a spin-orbit-coupling induced Mott insulator
journal, July 2014
- Dai, Jixia; Calleja, Eduardo; Cao, Gang
- Physical Review B, Vol. 90, Issue 4
Electron-doped : Evolution of a disordered Mott insulator into an exotic metallic state
journal, September 2010
- Korneta, O. B.; Qi, Tongfei; Chikara, S.
- Physical Review B, Vol. 82, Issue 11
Lattice-driven magnetoresistivity and metal-insulator transition in single-layered iridates
journal, September 2011
- Ge, M.; Qi, T. F.; Korneta, O. B.
- Physical Review B, Vol. 84, Issue 10
Spin-orbit tuned metal-insulator transitions in single-crystal Sr Ir Rh O ( )
journal, September 2012
- Qi, T. F.; Korneta, O. B.; Li, L.
- Physical Review B, Vol. 86, Issue 12
From insulator to -wave superconductor in single-crystal
journal, December 2015
- Yuan, S. J.; Aswartham, S.; Terzic, J.
- Physical Review B, Vol. 92, Issue 24
Twisted Hubbard Model for : Magnetism and Possible High Temperature Superconductivity
journal, March 2011
- Wang, Fa; Senthil, T.
- Physical Review Letters, Vol. 106, Issue 13
Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
journal, January 2009
- Jackeli, G.; Khaliullin, G.
- Physical Review Letters, Vol. 102, Issue 1
Microscopic Study of a Spin-Orbit-Induced Mott Insulator in Ir Oxides
journal, November 2010
- Watanabe, Hiroshi; Shirakawa, Tomonori; Yunoki, Seiji
- Physical Review Letters, Vol. 105, Issue 21
Pressure-induced insulating state in ( , Eu) single crystals
journal, January 2010
- Korneta, O. B.; Chikara, S.; Parkin, S.
- Physical Review B, Vol. 81, Issue 4
Observation of superconductivity and anomalous electrical resistivity in single-crystal Ir Te
journal, May 2013
- Li, L.; Qi, T. F.; Lin, L. S.
- Physical Review B, Vol. 87, Issue 17
Pressure Tuning of the Spin-Orbit Coupled Ground State in
journal, July 2012
- Haskel, D.; Fabbris, G.; Zhernenkov, Mikhail
- Physical Review Letters, Vol. 109, Issue 2
Giant magnetoelectric effect in the Mott insulator
journal, October 2009
- Chikara, S.; Korneta, O.; Crummett, W. P.
- Physical Review B, Vol. 80, Issue 14
Anomalous magnetic and transport behavior in the magnetic insulator
journal, December 2002
- Cao, G.; Xin, Y.; Alexander, C. S.
- Physical Review B, Vol. 66, Issue 21
Charge density wave formation accompanying ferromagnetic ordering in quasi-one-dimensional BaIrO3
journal, February 2000
- Cao, G.; Crow, J. E.; Guertin, R. P.
- Solid State Communications, Vol. 113, Issue 11
Observation of a metal-to-insulator transition with both Mott-Hubbard and Slater characteristics in Sr IrO from time-resolved photocarrier dynamics
journal, July 2012
- Hsieh, D.; Mahmood, F.; Torchinsky, D. H.
- Physical Review B, Vol. 86, Issue 3
A short history of SHELX
journal, December 2007
- Sheldrick, George M.
- Acta Crystallographica Section A Foundations of Crystallography, Vol. 64, Issue 1, p. 112-122
Recent advances in magnetic structure determination by neutron powder diffraction
journal, October 1993
- Rodríguez-Carvajal, Juan
- Physica B: Condensed Matter, Vol. 192, Issue 1-2
Multiple-scattering calculations of x-ray-absorption spectra
journal, July 1995
- Zabinsky, S. I.; Rehr, J. J.; Ankudinov, A.
- Physical Review B, Vol. 52, Issue 4
Simultaneous valence shift of Pr and Tb ions at the spin-state transition in (Pr Tb Ca CoO
journal, April 2013
- Fujishiro, H.; Naito, T.; Takeda, D.
- Physical Review B, Vol. 87, Issue 15
Different routes to pressure-induced volume collapse transitions in gadolinium and terbium metals
journal, December 2013
- Fabbris, G.; Matsuoka, T.; Lim, J.
- Physical Review B, Vol. 88, Issue 24
Structural and magnetic studies of
journal, April 1994
- Crawford, M. K.; Subramanian, M. A.; Harlow, R. L.
- Physical Review B, Vol. 49, Issue 13
Localized-to-itinerant electron transition in
journal, May 1994
- Cava, R. J.; Batlogg, B.; Kiyono, K.
- Physical Review B, Vol. 49, Issue 17
Magnetic and crystal structures of : A neutron diffraction study
journal, April 2013
- Ye, Feng; Chi, Songxue; Chakoumakos, Bryan C.
- Physical Review B, Vol. 87, Issue 14
Structure symmetry determination and magnetic evolution in
journal, November 2015
- Ye, Feng; Wang, Xiaoping; Hoffmann, Christina
- Physical Review B, Vol. 92, Issue 20
Structural Distortion-Induced Magnetoelastic Locking in Revealed through Nonlinear Optical Harmonic Generation
journal, March 2015
- Torchinsky, D. H.; Chu, H.; Zhao, L.
- Physical Review Letters, Vol. 114, Issue 9
Measurement of the internal magnetic field in the correlated iridates Ca IrO , Ca Ir O , Sr Ir O and Sr IrO
journal, March 2011
- Franke, I.; Baker, P. J.; Blundell, S. J.
- Physical Review B, Vol. 83, Issue 9
Mechanism for the metal-insulator transition in
journal, June 1995
- Carter, S. A.; Batlogg, B.; Cava, R. J.
- Physical Review B, Vol. 51, Issue 23
Metal-insulator transitions
journal, June 1991
- Paesler, Michael
- Journal of Non-Crystalline Solids, Vol. 130, Issue 1
Gate-defined Josephson junctions in magic-angle twisted bilayer graphene
journal, May 2021
- de Vries, Folkert K.; Portolés, Elías; Zheng, Giulia
- Nature Nanotechnology, Vol. 16, Issue 7
Atomically resolved spectroscopic study of Sr2IrO4: Experiment and theory
text, January 2013
- Li, Qing; Cao, Guixin; Okamoto, Satoshi
- ETH Zurich
Metal-insulator transitions
journal, January 1980
- Mott, N. F.
- Pure and Applied Chemistry, Vol. 52, Issue 1
Dimensionality controlled Mott transition and correlation effects in single- and bi-layer perovskite iridates
text, January 2012
- Wang, Q.; Cao, Y.; Waugh, J. A.
- arXiv
Different routes to pressure-induced volume collapse transitions in gadolinium and terbium metals
text, January 2013
- Fabbris, G.; Matsuoka, T.; Lim, J.
- arXiv
Works referencing / citing this record:
The challenge of spin–orbit-tuned ground states in iridates: a key issues review
journal, February 2018
- Cao, Gang; Schlottmann, Pedro
- Reports on Progress in Physics, Vol. 81, Issue 4
The J eff = 1/2 Antiferromagnet Sr 2 IrO 4 : A Golden Avenue toward New Physics and Functions
journal, October 2019
- Lu, Chengliang; Liu, Jun‐Ming
- Advanced Materials
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
- Wang, Ziyao; Wang, Baochen; Liu, Yangai
- Materials Research Express, Vol. 6, Issue 11
Synthesis and physical properties of the new iridium oxyfluoride using a topochemical reaction method
journal, January 2020
- Kuramochi, K.; Shimano, T.; Nishio, T.
- Physical Review Materials, Vol. 4, Issue 1
Decoupling of magnetism and electric transport in single-crystal (Sr1-xAx)2IrO4 (A = Ca or Ba)
text, January 2017
- Zhao, H. D.; Terzic, J.; Zheng, H.
- arXiv
The Jeff=1/2 antiferromagnet Sr2IrO4: A golden avenue toward new physics and functions
text, January 2021
- Lu, Chengliang; Liu, Jun-Ming
- arXiv