Atomic-scale observation of structural and electronic orders in the layered compound α-RuCl3
Abstract
A pseudospin-1/2 Mott phase on a honeycomb lattice is proposed to host the celebrated two-dimensional Kitaev model which has an elusive quantum spin liquid ground state, and fascinating physics relevant to the development of future templates towards topological quantum bits. Here we report a comprehensive, atomically resolved real-space study by scanning transmission electron and scanning tunnelling microscopies on a novel layered material displaying Kitaev physics, -RuCl3. Our local crystallography analysis reveals considerable variations in the geometry of the ligand sublattice in thin films of -RuCl3 that opens a way to realization of a spatially inhomogeneous magnetic ground state at the nanometre length scale. Using scanning tunnelling techniques, we observe the electronic energy gap of 0.25 eV and intra-unit cell symmetry breaking of charge distribution in individual -RuCl3 surface layer. The corresponding charge-ordered pattern has a fine structure associated with two different types of charge disproportionation at Cl-terminated surface.
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
- ORNL
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1337025
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 7; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Ziatdinov, Maxim A., Banerjee, Arnab, Maksov, Artem B., Berlijn, Tom, Zhou, Wu, Cao, Huibo, Yan, Jiaqiang, Bridges, Craig A., Mandrus, D. G., Nagler, Stephen E., Baddorf, Arthur P, and Kalinin, Sergei V. Atomic-scale observation of structural and electronic orders in the layered compound α-RuCl3. United States: N. p., 2016.
Web. doi:10.1038/ncomms13774.
Ziatdinov, Maxim A., Banerjee, Arnab, Maksov, Artem B., Berlijn, Tom, Zhou, Wu, Cao, Huibo, Yan, Jiaqiang, Bridges, Craig A., Mandrus, D. G., Nagler, Stephen E., Baddorf, Arthur P, & Kalinin, Sergei V. Atomic-scale observation of structural and electronic orders in the layered compound α-RuCl3. United States. https://doi.org/10.1038/ncomms13774
Ziatdinov, Maxim A., Banerjee, Arnab, Maksov, Artem B., Berlijn, Tom, Zhou, Wu, Cao, Huibo, Yan, Jiaqiang, Bridges, Craig A., Mandrus, D. G., Nagler, Stephen E., Baddorf, Arthur P, and Kalinin, Sergei V. 2016.
"Atomic-scale observation of structural and electronic orders in the layered compound α-RuCl3". United States. https://doi.org/10.1038/ncomms13774. https://www.osti.gov/servlets/purl/1337025.
@article{osti_1337025,
title = {Atomic-scale observation of structural and electronic orders in the layered compound α-RuCl3},
author = {Ziatdinov, Maxim A. and Banerjee, Arnab and Maksov, Artem B. and Berlijn, Tom and Zhou, Wu and Cao, Huibo and Yan, Jiaqiang and Bridges, Craig A. and Mandrus, D. G. and Nagler, Stephen E. and Baddorf, Arthur P and Kalinin, Sergei V},
abstractNote = {A pseudospin-1/2 Mott phase on a honeycomb lattice is proposed to host the celebrated two-dimensional Kitaev model which has an elusive quantum spin liquid ground state, and fascinating physics relevant to the development of future templates towards topological quantum bits. Here we report a comprehensive, atomically resolved real-space study by scanning transmission electron and scanning tunnelling microscopies on a novel layered material displaying Kitaev physics, -RuCl3. Our local crystallography analysis reveals considerable variations in the geometry of the ligand sublattice in thin films of -RuCl3 that opens a way to realization of a spatially inhomogeneous magnetic ground state at the nanometre length scale. Using scanning tunnelling techniques, we observe the electronic energy gap of 0.25 eV and intra-unit cell symmetry breaking of charge distribution in individual -RuCl3 surface layer. The corresponding charge-ordered pattern has a fine structure associated with two different types of charge disproportionation at Cl-terminated surface.},
doi = {10.1038/ncomms13774},
url = {https://www.osti.gov/biblio/1337025},
journal = {Nature Communications},
issn = {2041-1723},
number = ,
volume = 7,
place = {United States},
year = {Mon Dec 12 00:00:00 EST 2016},
month = {Mon Dec 12 00:00:00 EST 2016}
}
Web of Science
Figures / Tables:
Works referenced in this record:
Zigzag Magnetic Order in the Iridium Oxide
journal, February 2013
- Chaloupka, Jiří; Jackeli, George; Khaliullin, Giniyat
- Physical Review Letters, Vol. 110, Issue 9
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Atomic Structure and Superstructure ofα-RuCl3 by Scanning Tunneling Microscopy
journal, May 1990
- Cantow, Hans-Joachim; Hillebrecht, Harald; Magonov, Sergej N.
- Angewandte Chemie International Edition in English, Vol. 29, Issue 5
Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet
journal, April 2016
- Banerjee, A.; Bridges, C. A.; Yan, J. -Q.
- Nature Materials, Vol. 15, Issue 7
Monoclinic crystal structure of and the zigzag antiferromagnetic ground state
journal, December 2015
- Johnson, R. D.; Williams, S. C.; Haghighirad, A. A.
- Physical Review B, Vol. 92, Issue 23
Spin-Orbit Physics Giving Rise to Novel Phases in Correlated Systems: Iridates and Related Materials
journal, March 2016
- Rau, Jeffrey G.; Lee, Eric Kin-Ho; Kee, Hae-Young
- Annual Review of Condensed Matter Physics, Vol. 7, Issue 1
Strongly frustrated triangular spin lattice emerging from triplet dimer formation in honeycomb Li2IrO3
journal, January 2016
- Nishimoto, Satoshi; Katukuri, Vamshi M.; Yushankhai, Viktor
- Nature Communications, Vol. 7, Issue 1
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Magnetic order in : A honeycomb-lattice quantum magnet with strong spin-orbit coupling
journal, April 2015
- Sears, J. A.; Songvilay, M.; Plumb, K. W.
- Physical Review B, Vol. 91, Issue 14
Correlated Quantum Phenomena in the Strong Spin-Orbit Regime
journal, March 2014
- Witczak-Krempa, William; Chen, Gang; Kim, Yong Baek
- Annual Review of Condensed Matter Physics, Vol. 5, Issue 1
Unpaired Majorana modes in the gapped phase of Kitaev's honeycomb model
journal, October 2013
- Petrova, Olga; Mellado, Paula; Tchernyshyov, Oleg
- Physical Review B, Vol. 88, Issue 14
as a Novel Relativistic Mott Insulator with a 340-meV Gap
journal, December 2012
- Comin, R.; Levy, G.; Ludbrook, B.
- Physical Review Letters, Vol. 109, Issue 26
Special points for Brillouin-zone integrations
journal, June 1976
- Monkhorst, Hendrik J.; Pack, James D.
- Physical Review B, Vol. 13, Issue 12, p. 5188-5192
Order-by-disorder and spin-orbital liquids in a distorted Heisenberg-Kitaev model
journal, July 2014
- Sela, Eran; Jiang, Hong-Chen; Gerlach, Max H.
- Physical Review B, Vol. 90, Issue 3
Kitaev interactions between j = 1/2 moments in honeycomb Na 2 IrO 3 are large and ferromagnetic: insights from ab initio quantum chemistry calculations
journal, January 2014
- Katukuri, Vamshi M.; Nishimoto, S.; Yushankhai, V.
- New Journal of Physics, Vol. 16, Issue 1
Generic Spin Model for the Honeycomb Iridates beyond the Kitaev Limit
journal, February 2014
- Rau, Jeffrey G.; Lee, Eric Kin-Ho; Kee, Hae-Young
- Physical Review Letters, Vol. 112, Issue 7
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Big–deep–smart data in imaging for guiding materials design
journal, September 2015
- Kalinin, Sergei V.; Sumpter, Bobby G.; Archibald, Richard K.
- Nature Materials, Vol. 14, Issue 10
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
Phase instability induced by polar nanoregions in a relaxor ferroelectric system
journal, May 2008
- Xu, Guangyong; Wen, Jinsheng; Stock, C.
- Nature Materials, Vol. 7, Issue 7
Relevance of the Heisenberg-Kitaev Model for the Honeycomb Lattice Iridates
journal, March 2012
- Singh, Yogesh; Manni, S.; Reuther, J.
- Physical Review Letters, Vol. 108, Issue 12
Strong magnetic frustration and anti-site disorder causing spin-glass behavior in honeycomb Li2RhO3
journal, October 2015
- Katukuri, Vamshi M.; Nishimoto, Satoshi; Rousochatzakis, Ioannis
- Scientific Reports, Vol. 5, Issue 1
Kitaev magnetism in honeycomb with intermediate spin-orbit coupling
journal, June 2015
- Kim, Heung-Sik; V., Vijay Shankar; Catuneanu, Andrei
- Physical Review B, Vol. 91, Issue 24
Highly unconventional surface reconstruction of with persistent energy gap
journal, January 2015
- Lüpke, F.; Manni, S.; Erwin, S. C.
- Physical Review B, Vol. 91, Issue 4
Successive magnetic phase transitions in : XY-like frustrated magnet on the honeycomb lattice
journal, March 2015
- Kubota, Yumi; Tanaka, Hidekazu; Ono, Toshio
- Physical Review B, Vol. 91, Issue 9
Scattering Continuum and Possible Fractionalized Excitations in
journal, April 2015
- Sandilands, Luke J.; Tian, Yao; Plumb, Kemp W.
- Physical Review Letters, Vol. 114, Issue 14
: A spin-orbit assisted Mott insulator on a honeycomb lattice
journal, July 2014
- Plumb, K. W.; Clancy, J. P.; Sandilands, L. J.
- Physical Review B, Vol. 90, Issue 4
Identification of phases, symmetries and defects through local crystallography
journal, July 2015
- Belianinov, Alex; He, Qian; Kravchenko, Mikhail
- Nature Communications, Vol. 6, Issue 1
Majorana zero modes and topological quantum computation
journal, October 2015
- Sarma, Sankar Das; Freedman, Michael; Nayak, Chetan
- npj Quantum Information, Vol. 1, Issue 1
Angle-resolved photoemission study of the Kitaev candidate
journal, October 2016
- Zhou, Xiaoqing; Li, Haoxiang; Waugh, J. A.
- Physical Review B, Vol. 94, Issue 16
Big data and deep data in scanning and electron microscopies: deriving functionality from multidimensional data sets
journal, May 2015
- Belianinov, Alex; Vasudevan, Rama; Strelcov, Evgheni
- Advanced Structural and Chemical Imaging, Vol. 1, Issue 1
Kitaev exchange and field-induced quantum spin-liquid states in honeycomb α-RuCl3
journal, November 2016
- Yadav, Ravi; Bogdanov, Nikolay A.; Katukuri, Vamshi M.
- Scientific Reports, Vol. 6, Issue 1
Crystal structure and magnetism in : An ab initio study
journal, April 2016
- Kim, Heung-Sik; Kee, Hae-Young
- Physical Review B, Vol. 93, Issue 15
Optical and transport properties of the magnetic semiconductor α-RuCl3
journal, March 1971
- Binotto, L.; Pollini, I.; Spinolo, G.
- Physica Status Solidi (b), Vol. 44, Issue 1
Magnetic Properties of Restacked 2D Spin 1/2 honeycomb RuCl 3 Nanosheets
journal, May 2016
- Weber, Daniel; Schoop, Leslie M.; Duppel, Viola
- Nano Letters, Vol. 16, Issue 6
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
Direct evidence for dominant bond-directional interactions in a honeycomb lattice iridate Na2IrO3
journal, May 2015
- Hwan Chun, Sae; Kim, Jong-Woo; Kim, Jungho
- Nature Physics, Vol. 11, Issue 6
Quantum Spin Hall Effect in a Transition Metal Oxide
journal, June 2009
- Shitade, Atsuo; Katsura, Hosho; Kuneš, Jan
- Physical Review Letters, Vol. 102, Issue 25
Quantum phase transition from triangular to stripe charge order in NbSe2
journal, January 2013
- Soumyanarayanan, A.; Yee, M. M.; He, Y.
- Proceedings of the National Academy of Sciences, Vol. 110, Issue 5
Possible proximity of the Mott insulating iridate Na IrO to a topological phase: Phase diagram of the Heisenberg-Kitaev model in a magnetic field
journal, June 2011
- Jiang, Hong-Chen; Gu, Zheng-Cheng; Qi, Xiao-Liang
- Physical Review B, Vol. 83, Issue 24
Visualizing pair formation on the atomic scale in the high-Tc superconductor Bi2Sr2CaCu2O8+δ
journal, May 2007
- Gomes, Kenjiro K.; Pasupathy, Abhay N.; Pushp, Aakash
- Nature, Vol. 447, Issue 7144
Low-temperature crystal and magnetic structure of
journal, April 2016
- Cao, H. B.; Banerjee, A.; Yan, J. -Q.
- Physical Review B, Vol. 93, Issue 13
Magnetic Properties of Restacked 2D Spin 1/2 honeycomb RuCl 3 Nanosheets
journal, May 2016
- Weber, Daniel; Schoop, Leslie M.; Duppel, Viola
- Nano Letters, Vol. 16, Issue 6
Identification of phases, symmetries and defects through local crystallography
journal, July 2015
- Belianinov, Alex; He, Qian; Kravchenko, Mikhail
- Nature Communications, Vol. 6, Issue 1
Big–deep–smart data in imaging for guiding materials design
journal, September 2015
- Kalinin, Sergei V.; Sumpter, Bobby G.; Archibald, Richard K.
- Nature Materials, Vol. 14, Issue 10
Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet
journal, April 2016
- Banerjee, A.; Bridges, C. A.; Yan, J. -Q.
- Nature Materials, Vol. 15, Issue 7
Kitaev exchange and field-induced quantum spin-liquid states in honeycomb α-RuCl3
journal, November 2016
- Yadav, Ravi; Bogdanov, Nikolay A.; Katukuri, Vamshi M.
- Scientific Reports, Vol. 6, Issue 1
Electronic properties of the narrow-band material α-
journal, May 1996
- Pollini, I.
- Physical Review B, Vol. 53, Issue 19
Landau Levels of Majorana Fermions in a Spin Liquid
journal, April 2016
- Rachel, Stephan; Fritz, Lars; Vojta, Matthias
- Physical Review Letters, Vol. 116, Issue 16
Big data and deep data in scanning and electron microscopies: deriving functionality from multidimensional data sets
journal, May 2015
- Belianinov, Alex; Vasudevan, Rama; Strelcov, Evgheni
- Advanced Structural and Chemical Imaging, Vol. 1, Issue 1
Relevance of the Heisenberg-Kitaev model for the honeycomb lattice iridates A_2IrO_3
text, January 2011
- Singh, Yogesh; Manni, S.; Reuther, J.
- arXiv
A quantum phase transition from triangular to stripe charge order in NbSe$_{2}$
text, January 2012
- Soumyanarayanan, Anjan; Yee, Michael M.; He, Yang
- arXiv
Generic spin model for the honeycomb iridates beyond the Kitaev limit
text, January 2013
- Rau, Jeffrey G.; Lee, Eric Kin-Ho; Kee, Hae-Young
- arXiv
Strong magnetic frustration and anti-site disorder causing spin-glass behavior in honeycomb Li2RhO3
text, January 2015
- Katukuri, Vamshi M.; Nishimoto, Satoshi; Rousochatzakis, Ioannis
- arXiv
Works referencing / citing this record:
Electronic and magnetic properties of monolayer α-RuCl 3 : a first-principles and Monte Carlo study
journal, January 2018
- Sarikurt, S.; Kadioglu, Y.; Ersan, F.
- Physical Chemistry Chemical Physics, Vol. 20, Issue 2
High-temperature Dirac half-metal PdCl 3 : a promising candidate for realizing quantum anomalous Hall effect
journal, January 2018
- Wang, Ya-ping; Li, Sheng-shi; Zhang, Chang-wen
- Journal of Materials Chemistry C, Vol. 6, Issue 38
Strain effects on electronic and magnetic properties of the monolayer α - RuCl 3: A first-principles and Monte Carlo study
journal, February 2019
- Vatansever, Erol; Sarikurt, Sevil; Ersan, Fatih
- Journal of Applied Physics, Vol. 125, Issue 8
Models and materials for generalized Kitaev magnetism
journal, November 2017
- Winter, Stephen M.; Tsirlin, Alexander A.; Daghofer, Maria
- Journal of Physics: Condensed Matter, Vol. 29, Issue 49
Antiferromagnetic spin-frustrated layers of corner-sharing Cu 4 tetrahedra on the kagome lattice in volcanic minerals Cu 5 O 2 (VO 4 ) 2 (CuCl), NaCu 5 O 2 (SeO 3 ) 2 Cl 3 , and K 2 Cu 5 Cl 8 (OH) 4 ·2H 2 O
journal, September 2018
- Volkova, L. M.; Marinin, D. V.
- Journal of Physics: Condensed Matter, Vol. 30, Issue 42
Sub-gap optical response in the Kitaev spin-liquid candidate α -RuCl 3
journal, November 2018
- Reschke, Stephan; Mayr, Franz; Widmann, Sebastian
- Journal of Physics: Condensed Matter, Vol. 30, Issue 47
Evidence for charge transfer and proximate magnetism in graphene– heterostructures
journal, October 2019
- Zhou, Boyi; Balgley, J.; Lampen-Kelley, P.
- Physical Review B, Vol. 100, Issue 16
Field-induced quantum criticality in the Kitaev system
journal, July 2017
- Wolter, A. U. B.; Corredor, L. T.; Janssen, L.
- Physical Review B, Vol. 96, Issue 4
Electronically highly cubic conditions for Ru in
journal, October 2017
- Agrestini, S.; Kuo, C. -Y.; Ko, K. -T.
- Physical Review B, Vol. 96, Issue 16
Interlayer coupling effect on a bilayer Kitaev model
journal, March 2018
- Tomishige, Hiroyuki; Nasu, Joji; Koga, Akihisa
- Physical Review B, Vol. 97, Issue 9
Field evolution of magnons in by high-resolution polarized terahertz spectroscopy
journal, September 2018
- Wu, Liang; Little, A.; Aldape, E. E.
- Physical Review B, Vol. 98, Issue 9
Antiferromagnetic Resonance and Terahertz Continuum in
journal, November 2017
- Little, A.; Wu, Liang; Lampen-Kelley, P.
- Physical Review Letters, Vol. 119, Issue 22
Approximately Quantized Thermal Hall Effect of Chiral Liquids Coupled to Phonons
journal, August 2018
- Vinkler-Aviv, Yuval; Rosch, Achim
- Physical Review X, Vol. 8, Issue 3
Magnon Transport in Quasi-Two-Dimensional van der Waals Antiferromagnets
journal, February 2019
- Xing, Wenyu; Qiu, Luyi; Wang, Xirui
- Physical Review X, Vol. 9, Issue 1
Pressure tuning of charge ordering in iron oxide
text, January 2018
- Ovsyannikov, Sergey; Bykov, Maxim; Bykova, Elena
- Deutsches Elektronen-Synchrotron, DESY, Hamburg
Pressure tuning of charge ordering in iron oxide
journal, October 2018
- Ovsyannikov, Sergey V.; Bykov, Maxim; Bykova, Elena
- Nature Communications, Vol. 9, Issue 1
Models and Materials for Generalized Kitaev Magnetism
text, January 2017
- Winter, Stephen M.; Tsirlin, Alexander A.; Daghofer, Maria
- arXiv
Electronic and magnetic properties of the monolayer RuCl$_3$: A first-principles and Monte Carlo study
text, January 2017
- Sarikurt, S.; Kadioglu, Y.; Ersan, F.
- arXiv
Interlayer Coupling Effect on a Bilayer Kitaev Model
text, January 2017
- Tomishige, Hiroyuki; Nasu, Joji; Koga, Akihisa
- arXiv
Magnon transport in quasi-two-dimensional van der Waals antiferromagnets
text, January 2019
- Xing, Wenyu; Qiu, Luyi; Wang, Xirui
- arXiv
Pressure tuning of charge ordering in iron oxide
journal, October 2018
- Ovsyannikov, Sergey V.; Bykov, Maxim; Bykova, Elena
- Nature Communications, Vol. 9, Issue 1
Ordered states in the Kitaev-Heisenberg model: From 1D chains to 2D honeycomb
text, January 2018
- Agrapidis, Cliò Efthimia; Van Den Brink, Jeroen; Nishimoto, Satoshi
- London : Nature Publishing Group
Evidence for charge transfer and proximate magnetism in graphene/a-RuCl_3 heterostructures
text, January 2018
- Zhou, Boyi; Balgley, J.; Lampen-Kelley, P.
- arXiv
Figures / Tables found in this record: