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Title: 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:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [2];  [1];  [3];  [3]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
  3. 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}
}

Journal Article:
Free Publicly Available Full Text
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Citation Metrics:
Cited by: 56 works
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Figures / Tables:

Figure 1 Figure 1: Scanning transmission electron microscopy data on $$\alpha$$-RuCl3 films. (a) Z-contrast STEM image of $$\alpha$$-RuCl3 film (raw data). Inset shows filtered data, where brown and blue crosses correspond to the centers of Ru/Cl columns and Cl columns, respectively. (b,c) Histogram-based visualization of inter-column distances for six nearest neighbours ofmore » Ru/Cl columns (b) and Cl columns (c). Dotted red vertical lines show the value of inter-column distances expected for perfect trigonal symmetry. The red arrow in c indicates the presence of a well-defined shoulder originating from an increase in nearest neighbour distances of Cl columns. (d) Line profile illustrating a modulation of inter-column distances for Cl and Ru/Cl columns with respect to the value of 198 pm for ideal trigonal symmetry.« less

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Angle-resolved photoemission study of the Kitaev candidate α RuCl 3
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Big data and deep data in scanning and electron microscopies: deriving functionality from multidimensional data sets
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Kitaev exchange and field-induced quantum spin-liquid states in honeycomb α-RuCl3
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Magnetic Properties of Restacked 2D Spin 1/2 honeycomb RuCl 3 Nanosheets
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Big–deep–smart data in imaging for guiding materials design
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Works referencing / citing this record:

Electronic and magnetic properties of monolayer α-RuCl 3 : a first-principles and Monte Carlo study
journal, January 2018


High-temperature Dirac half-metal PdCl 3 : a promising candidate for realizing quantum anomalous Hall effect
journal, January 2018


Strain effects on electronic and magnetic properties of the monolayer α - RuCl 3: A first-principles and Monte Carlo study
journal, February 2019


Models and materials for generalized Kitaev magnetism
journal, November 2017


Sub-gap optical response in the Kitaev spin-liquid candidate α -RuCl 3
journal, November 2018


Evidence for charge transfer and proximate magnetism in graphene– α RuCl 3 heterostructures
journal, October 2019


Field-induced quantum criticality in the Kitaev system α RuCl 3
journal, July 2017


Electronically highly cubic conditions for Ru in α RuCl 3
journal, October 2017


Interlayer coupling effect on a bilayer Kitaev model
journal, March 2018


Field evolution of magnons in α RuCl 3 by high-resolution polarized terahertz spectroscopy
journal, September 2018


Antiferromagnetic Resonance and Terahertz Continuum in α RuCl 3
journal, November 2017


Approximately Quantized Thermal Hall Effect of Chiral Liquids Coupled to Phonons
journal, August 2018


Magnon Transport in Quasi-Two-Dimensional van der Waals Antiferromagnets
journal, February 2019


Pressure tuning of charge ordering in iron oxide
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Pressure tuning of charge ordering in iron oxide
journal, October 2018


Models and Materials for Generalized Kitaev Magnetism
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Interlayer Coupling Effect on a Bilayer Kitaev Model
text, January 2017


Pressure tuning of charge ordering in iron oxide
journal, October 2018


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text, January 2018


Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.