Honeycomb lattice Na2IrO3 at high pressures: A robust spin-orbit Mott insulator

Xi, Xiaoxiang; Bo, Xiangyan; Xu, X. S.; Kong, P. P.; Liu, Z.; Hong, X. G.; Jin, C. Q.; Cao, G.; Wan, Xiangang; Carr, G. L.

doi:10.1103/PhysRevB.98.125117

Honeycomb lattice ${Na}_{2} {IrO}_{3}$ at high pressures: A robust spin-orbit Mott insulator

Journal Article · Mon Sep 10 00:00:00 EDT 2018 · Physical Review B

DOI:https://doi.org/10.1103/PhysRevB.98.125117· OSTI ID:1483240

Xi, Xiaoxiang ^[1]; Bo, Xiangyan ^[2]; Xu, X. S. ^[3]; Kong, P. P. ^[4]; Liu, Z. ^[5]; Hong, X. G. ^[6]; Jin, C. Q. ^[4]; Cao, G. ^[7]; Wan, Xiangang ^[2]; Carr, G. L. ^[8]

Nanjing Univ., Nanjing (China); Brookhaven National Lab. (BNL), Upton, NY (United States)
Nanjing Univ., Nanjing (China)
Univ. of Nebraska, Lincoln, NE (United States)
Chinese Academy of Sciences (CAS), Beijing (China)
The George Washington Univ., Washington, DC (United States)
Stony Brook Univ., Stony Brook, NY (United States); Center for High Pressure Science and Technology Advanced Research, Beijing (China)
Univ. of Colorado at Boulder, Boulder, CO (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)

The honeycomb iridate Na₂IrO₃ has received much attention as a candidate to realize a quantum spin liquid state, but the nature of its insulating state remains controversial. We found that the material exhibits structural transitions at 3 and 10 GPa. The former is accompanied by 166-meV suppression of the activation gap, but the energies for the low-lying interband transitions change by less than 10 meV. This can be reconciled in a picture in which the application of high pressure barely shifts the electronic bands, but rather merely broadens them. First-principles calculations uncover a strong correlation between the band gap and the β angle of the monoclinic structure, indicating non-negligible interlayer coupling. Furthermore, these results offer clear evidence for a spin-orbit Mott insulating state in Na₂IrO₃ and are inconsistent with the quasimolecular orbital model.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC02-98CH10886; SC0012704

OSTI ID:: 1483240

Alternate ID(s):: OSTI ID: 1469262

Report Number(s):: BNL--209471-2018-JAAM

Journal Information:: Physical Review B, Journal Name: Physical Review B Journal Issue: 12 Vol. 98; ISSN 2469-9950; ISSN PRBMDO

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (55)

Anyons in an exactly solved model and beyond Kitaev, Alexei Annals of Physics, Vol. 321, Issue 1 https://doi.org/10.1016/j.aop.2005.10.005	journal	January 2006
Pressure-enhanced Insulating State and Trigonal Distortion Relaxation in Geometrically Frustrated Pyrochlore Eu ₂ Sn ₂ O ₇ Zhao, Yongsheng; Yang, Wenge; Li, Nana The Journal of Physical Chemistry C, Vol. 120, Issue 17 https://doi.org/10.1021/acs.jpcc.6b02246	journal	April 2016
Mott physics and band topology in materials with strong spin–orbit interaction Pesin, Dmytro; Balents, Leon Nature Physics, Vol. 6, Issue 5 https://doi.org/10.1038/nphys1606	journal	March 2010
Direct evidence for dominant bond-directional interactions in a honeycomb lattice iridate Na2IrO3 Hwan Chun, Sae; Kim, Jong-Woo; Kim, Jungho Nature Physics, Vol. 11, Issue 6 https://doi.org/10.1038/nphys3322	journal	May 2015
Pressure-driven collapse of the relativistic electronic ground state in a honeycomb iridate Clancy, J. Patrick; Gretarsson, Hlynur; Sears, Jennifer A. npj Quantum Materials, Vol. 3, Issue 1 https://doi.org/10.1038/s41535-018-0109-0	journal	August 2018
Recent progress on correlated electron systems with strong spin–orbit coupling Schaffer, Robert; Kin-Ho Lee, Eric; Yang, Bohm-Jung Reports on Progress in Physics, Vol. 79, Issue 9 https://doi.org/10.1088/0034-4885/79/9/094504	journal	August 2016
The challenge of spin–orbit-tuned ground states in iridates: a key issues review Cao, Gang; Schlottmann, Pedro Reports on Progress in Physics, Vol. 81, Issue 4 https://doi.org/10.1088/1361-6633/aaa979	journal	February 2018
Spin–orbital locking, emergent pseudo-spin and magnetic order in honeycomb lattice iridates Bhattacharjee, Subhro; Lee, Sung-Sik; Kim, Yong Baek New Journal of Physics, Vol. 14, Issue 7 https://doi.org/10.1088/1367-2630/14/7/073015	journal	July 2012
Kitaev interactions between j = 1/2 moments in honeycomb Na ₂ IrO ₃ are large and ferromagnetic: insights from ab initio quantum chemistry calculations Katukuri, Vamshi M.; Nishimoto, S.; Yushankhai, V. New Journal of Physics, Vol. 16, Issue 1 https://doi.org/10.1088/1367-2630/16/1/013056	journal	January 2014
Temperature dependence of the electronic structure of the J eff = 1 2 Mott insulator Sr 2 IrO 4 studied by optical spectroscopy Moon, S. J.; Jin, Hosub; Choi, W. S. Physical Review B, Vol. 80, Issue 19 https://doi.org/10.1103/PhysRevB.80.195110	journal	November 2009
Topological semimetal and Fermi-arc surface states in the electronic structure of pyrochlore iridates Wan, Xiangang; Turner, Ari M.; Vishwanath, Ashvin Physical Review B, Vol. 83, Issue 20 https://doi.org/10.1103/PhysRevB.83.205101	journal	May 2011
Long-range magnetic ordering in Na 2 IrO 3 Liu, X.; Berlijn, T.; Yin, W. -G. Physical Review B, Vol. 83, Issue 22 https://doi.org/10.1103/PhysRevB.83.220403	journal	June 2011
Finite-temperature phase diagram of the Heisenberg-Kitaev model Reuther, Johannes; Thomale, Ronny; Trebst, Simon Physical Review B, Vol. 84, Issue 10 https://doi.org/10.1103/PhysRevB.84.100406	journal	September 2011
Kitaev-Heisenberg- J 2 - J 3 model for the iridates A 2 IrO 3 Kimchi, Itamar; You, Yi-Zhuang Physical Review B, Vol. 84, Issue 18 https://doi.org/10.1103/PhysRevB.84.180407	journal	November 2011
Direct evidence of a zigzag spin-chain structure in the honeycomb lattice: A neutron and x-ray diffraction investigation of single-crystal Na 2 IrO 3 Ye, Feng; Chi, Songxue; Cao, Huibo Physical Review B, Vol. 85, Issue 18 https://doi.org/10.1103/PhysRevB.85.180403	journal	May 2012
Strain-induced topological insulator phase and effective magnetic interactions in Li 2 IrO 3 Kim, Heung-Sik; Kim, Choong H.; Jeong, Hogyun Physical Review B, Vol. 87, Issue 16 https://doi.org/10.1103/PhysRevB.87.165117	journal	April 2013
Magnetic excitation spectrum of Na 2 IrO 3 probed with resonant inelastic x-ray scattering Gretarsson, H.; Clancy, J. P.; Singh, Yogesh Physical Review B, Vol. 87, Issue 22 https://doi.org/10.1103/PhysRevB.87.220407	journal	June 2013
Ab initio analysis of the tight-binding parameters and magnetic interactions in Na 2 IrO 3 Foyevtsova, Kateryna; Jeschke, Harald O.; Mazin, I. I. Physical Review B, Vol. 88, Issue 3 https://doi.org/10.1103/PhysRevB.88.035107	journal	July 2013
Mixing between J eff = 1 2 and 3 2 orbitals in Na 2 IrO 3 : A spectroscopic and density functional calculation study Sohn, C. H.; Kim, H. -S.; Qi, T. F. Physical Review B, Vol. 88, Issue 8 https://doi.org/10.1103/PhysRevB.88.085125	journal	August 2013
Evolution of magnetism in the single-crystal honeycomb iridates ( Na 1 − x Li x ) 2 Ir O 3 Cao, G.; Qi, T. F.; Li, L. Physical Review B, Vol. 88, Issue 22 https://doi.org/10.1103/PhysRevB.88.220414	journal	December 2013
Importance of anisotropic exchange interactions in honeycomb iridates: Minimal model for zigzag antiferromagnetic order in Na 2 IrO 3 Sizyuk, Yuriy; Price, Craig; Wölfle, Peter Physical Review B, Vol. 90, Issue 15 https://doi.org/10.1103/PhysRevB.90.155126	journal	October 2014
Analysis of the optical conductivity for A 2 IrO 3 ( A = Na , Li ) from first principles Li, Ying; Foyevtsova, Kateryna; Jeschke, Harald O. Physical Review B, Vol. 91, Issue 16 https://doi.org/10.1103/PhysRevB.91.161101	journal	April 2015
Dynamical properties of the honeycomb-lattice iridates Na 2 IrO 3 Suzuki, Takafumi; Yamada, Takuto; Yamaji, Youhei Physical Review B, Vol. 92, Issue 18 https://doi.org/10.1103/PhysRevB.92.184411	journal	November 2015
Cd 2 Re 2 O 7 under high pressure: Pyrochlore lattice distortion-driven metal-to-nonmetal transition Malavi, Pallavi S.; Karmakar, S.; Sharma, S. M. Physical Review B, Vol. 93, Issue 3 https://doi.org/10.1103/PhysRevB.93.035139	journal	January 2016
Clues and criteria for designing a Kitaev spin liquid revealed by thermal and spin excitations of the honeycomb iridate Na 2 IrO 3 Yamaji, Youhei; Suzuki, Takafumi; Yamada, Takuto Physical Review B, Vol. 93, Issue 17 https://doi.org/10.1103/PhysRevB.93.174425	journal	May 2016
High-pressure versus isoelectronic doping effect on the honeycomb iridate Na 2 IrO 3 Hermann, V.; Ebad-Allah, J.; Freund, F. Physical Review B, Vol. 96, Issue 19 https://doi.org/10.1103/PhysRevB.96.195137	journal	November 2017
Competition between spin-orbit coupling, magnetism, and dimerization in the honeycomb iridates: α − Li 2 IrO 3 under pressure Hermann, V.; Altmeyer, M.; Ebad-Allah, J. Physical Review B, Vol. 97, Issue 2 https://doi.org/10.1103/PhysRevB.97.020104	journal	January 2018
Detuning the honeycomb of α − RuCl 3 : Pressure-dependent optical studies reveal broken symmetry Biesner, Tobias; Biswas, Sananda; Li, Weiwu Physical Review B, Vol. 97, Issue 22 https://doi.org/10.1103/PhysRevB.97.220401	journal	June 2018
Pressure-induced dimerization and valence bond crystal formation in the Kitaev-Heisenberg magnet α − RuCl 3 Bastien, G.; Garbarino, G.; Yadav, R. Physical Review B, Vol. 97, Issue 24 https://doi.org/10.1103/PhysRevB.97.241108	journal	June 2018
Novel J eff = 1 / 2 Mott State Induced by Relativistic Spin-Orbit Coupling in Sr 2 IrO 4 Kim, B. J.; Jin, Hosub; Moon, S. J. Physical Review Letters, Vol. 101, Issue 7 https://doi.org/10.1103/PhysRevLett.101.076402	journal	August 2008
Dimensionality-Controlled Insulator-Metal Transition and Correlated Metallic State in 5 d Transition Metal Oxides Sr n + 1 Ir n O 3 n + 1 ( n = 1 , 2, and ∞ ) Moon, S. J.; Jin, H.; Kim, K. W. Physical Review Letters, Vol. 101, Issue 22 https://doi.org/10.1103/PhysRevLett.101.226402	journal	November 2008
Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models Jackeli, G.; Khaliullin, G. Physical Review Letters, Vol. 102, Issue 1 https://doi.org/10.1103/PhysRevLett.102.017205	journal	January 2009
Quantum Spin Hall Effect in a Transition Metal Oxide Na 2 IrO 3 Shitade, Atsuo; Katsura, Hosho; Kuneš, Jan Physical Review Letters, Vol. 102, Issue 25 https://doi.org/10.1103/PhysRevLett.102.256403	journal	June 2009
Kitaev-Heisenberg Model on a Honeycomb Lattice: Possible Exotic Phases in Iridium Oxides A 2 IrO 3 Chaloupka, Jiří; Jackeli, George; Khaliullin, Giniyat Physical Review Letters, Vol. 105, Issue 2 https://doi.org/10.1103/PhysRevLett.105.027204	journal	July 2010
Microscopic Study of a Spin-Orbit-Induced Mott Insulator in Ir Oxides Watanabe, Hiroshi; Shirakawa, Tomonori; Yunoki, Seiji Physical Review Letters, Vol. 105, Issue 21 https://doi.org/10.1103/PhysRevLett.105.216410	journal	November 2010
Topological Quantum Phase Transition in 5 d Transition Metal Oxide Na 2 IrO 3 Kim, Choong H.; Kim, Heung Sik; Jeong, Hogyun Physical Review Letters, Vol. 108, Issue 10 https://doi.org/10.1103/PhysRevLett.108.106401	journal	March 2012
Relevance of the Heisenberg-Kitaev Model for the Honeycomb Lattice Iridates A 2 IrO 3 Singh, Yogesh; Manni, S.; Reuther, J. Physical Review Letters, Vol. 108, Issue 12 https://doi.org/10.1103/PhysRevLett.108.127203	journal	March 2012
Spin Waves and Revised Crystal Structure of Honeycomb Iridate Na 2 IrO 3 Choi, S. K.; Coldea, R.; Kolmogorov, A. N. Physical Review Letters, Vol. 108, Issue 12 https://doi.org/10.1103/PhysRevLett.108.127204	journal	March 2012
Pressure Tuning of the Spin-Orbit Coupled Ground State in Sr 2 IrO 4 Haskel, D.; Fabbris, G.; Zhernenkov, Mikhail Physical Review Letters, Vol. 109, Issue 2 https://doi.org/10.1103/PhysRevLett.109.027204	journal	July 2012
Testing the Validity of the Strong Spin-Orbit-Coupling Limit for Octahedrally Coordinated Iridate Compounds in a Model System Sr 3 CuIrO 6 Liu, X.; Katukuri, Vamshi M.; Hozoi, L. Physical Review Letters, Vol. 109, Issue 15 https://doi.org/10.1103/PhysRevLett.109.157401	journal	October 2012
Critical Properties of the Kitaev-Heisenberg Model Price, Craig C.; Perkins, Natalia B. Physical Review Letters, Vol. 109, Issue 18 https://doi.org/10.1103/PhysRevLett.109.187201	journal	November 2012
Na 2 IrO 3 as a Molecular Orbital Crystal Mazin, I. I.; Jeschke, Harald O.; Foyevtsova, Kateryna Physical Review Letters, Vol. 109, Issue 19 https://doi.org/10.1103/PhysRevLett.109.197201	journal	November 2012
Na 2 IrO 3 as a Novel Relativistic Mott Insulator with a 340-meV Gap Comin, R.; Levy, G.; Ludbrook, B. Physical Review Letters, Vol. 109, Issue 26 https://doi.org/10.1103/PhysRevLett.109.266406	journal	December 2012
Crystal-Field Splitting and Correlation Effect on the Electronic Structure of A 2 IrO 3 Gretarsson, H.; Clancy, J. P.; Liu, X. Physical Review Letters, Vol. 110, Issue 7 https://doi.org/10.1103/PhysRevLett.110.076402	journal	February 2013
Zigzag Magnetic Order in the Iridium Oxide Na 2 IrO 3 Chaloupka, Jiří; Jackeli, George; Khaliullin, Giniyat Physical Review Letters, Vol. 110, Issue 9 https://doi.org/10.1103/PhysRevLett.110.097204	journal	February 2013
Signatures of a Pressure-Induced Topological Quantum Phase Transition in BiTeI Xi, Xiaoxiang; Ma, Chunli; Liu, Zhenxian Physical Review Letters, Vol. 111, Issue 15 https://doi.org/10.1103/PhysRevLett.111.155701	journal	October 2013
Generic Spin Model for the Honeycomb Iridates beyond the Kitaev Limit Rau, Jeffrey G.; Lee, Eric Kin-Ho; Kee, Hae-Young Physical Review Letters, Vol. 112, Issue 7 https://doi.org/10.1103/PhysRevLett.112.077204	journal	February 2014
First-Principles Study of the Honeycomb-Lattice Iridates Na 2 IrO 3 in the Presence of Strong Spin-Orbit Interaction and Electron Correlations Yamaji, Youhei; Nomura, Yusuke; Kurita, Moyuru Physical Review Letters, Vol. 113, Issue 10 https://doi.org/10.1103/PhysRevLett.113.107201	journal	September 2014
First-Principles Study of the Magnetic Structure of Na 2 IrO 3 Hu, Kaige; Wang, Fa; Feng, Ji Physical Review Letters, Vol. 115, Issue 16 https://doi.org/10.1103/PhysRevLett.115.167204	journal	October 2015
From a Quasimolecular Band Insulator to a Relativistic Mott Insulator in t 2 g 5 Systems with a Honeycomb Lattice Structure Kim, Beom Hyun; Shirakawa, Tomonori; Yunoki, Seiji Physical Review Letters, Vol. 117, Issue 18 https://doi.org/10.1103/PhysRevLett.117.187201	journal	October 2016
VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data Momma, Koichi; Izumi, Fujio Journal of Applied Crystallography, Vol. 44, Issue 6 https://doi.org/10.1107/S0021889811038970	journal	October 2011
Phase-Sensitive Observation of a Spin-Orbital Mott State in Sr2IrO4 Kim, B. J.; Ohsumi, H.; Komesu, T. Science, Vol. 323, Issue 5919 https://doi.org/10.1126/science.1167106	journal	March 2009
Frontiers of 4d- and 5d-Transition Metal Oxides Cao, Gang; De-Long, Lance https://doi.org/10.1142/8331	book	November 2011
Correlated Quantum Phenomena in the Strong Spin-Orbit Regime Witczak-Krempa, William; Chen, Gang; Kim, Yong Baek Annual Review of Condensed Matter Physics, Vol. 5, Issue 1 https://doi.org/10.1146/annurev-conmatphys-020911-125138	journal	March 2014
Spin-Orbit Physics Giving Rise to Novel Phases in Correlated Systems: Iridates and Related Materials Rau, Jeffrey G.; Lee, Eric Kin-Ho; Kee, Hae-Young Annual Review of Condensed Matter Physics, Vol. 7, Issue 1 https://doi.org/10.1146/annurev-conmatphys-031115-011319	journal	March 2016

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Honeycomb lattice ${Na}_{2} {IrO}_{3}$ at high pressures: A robust spin-orbit Mott insulator