Crystal Structure Reconstruction in the Surface Monolayer of the Quantum Spin Liquid Candidate α-RuCl3
Abstract
α-RuCl3, a layered 2D material, was recently identified as a promising candidate for realizing a Kitaev quantum spin liquid. However one fundamental property, the crystal structure, has not been well resolved yet due to difficulty of bulk diffraction techniques caused by layer stacking faults. Furthermore, the surface relaxation of monolayer-level thin films is completely unknown yet. In this report, surface sensitive low energy electron diffraction technique with µm selectivity (µ-LEED) combined with dynamical LEED analysis were used to reveal the detailed crystal structure of the surface monolayer of α-RuCl3. A surface structural distortion that breaks the inversion symmetry of the ideal bulk structure was revealed. To be specific, we found the surface Cl sub-lattice is buckled with one Cl atom approximately 0.16 Å below the other two Cl atoms, in the unit cell. The Ru atomic layer shows an even larger buckling of approximately 0.31 Å. Through density functional theory (DFT) calculations, we suggested that this surface distortion may be induced by Cl-vacancies that are inevitable in this material system. Inversion symmetry breaking in this material could have a significant impact on the 2D Kitaev interaction for both, interfaces with other 2D materials, such as graphene and future monolayer devices.
- Authors:
-
[1];
[4];
[1]
- Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
- Univ. of New Hampshire, Durham, NH (United States); Univ. of Florida, Gainesville, FL (United States)
- Washington Univ., St. Louis, MO (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division; Univ. of Tennessee, Knoxville, TN (United States)
- Univ. of New Hampshire, Durham, NH (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN) and National Synchrotron Light Source II (NSLS-II); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- National Science Foundation (NSF); Gordon and Betty Moore Foundation; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1604620
- Alternate Identifier(s):
- OSTI ID: 1649057
- Report Number(s):
- BNL-213716-2020-JAAM
Journal ID: ISSN 2053-1583
- Grant/Contract Number:
- SC0012704; TG-PHY170023; PHY-1229408; GBMF4416; AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- 2D Materials
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 3; Journal ID: ISSN 2053-1583
- Publisher:
- IOP Publishing
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Dai, Zhongwei, Yu, Jie-Xiang, Zhou, Boyi, Tenney, Samuel, Lampen-Kelley, Paula, Yan, Jiaqiang, Mandrus, David G., Henriksen, Erik, Zang, Jiadong, Pohl, Karsten, and Sadowski, Jerzy T. Crystal Structure Reconstruction in the Surface Monolayer of the Quantum Spin Liquid Candidate α-RuCl3. United States: N. p., 2020.
Web. doi:10.1088/2053-1583/ab7e0e.
Dai, Zhongwei, Yu, Jie-Xiang, Zhou, Boyi, Tenney, Samuel, Lampen-Kelley, Paula, Yan, Jiaqiang, Mandrus, David G., Henriksen, Erik, Zang, Jiadong, Pohl, Karsten, & Sadowski, Jerzy T. Crystal Structure Reconstruction in the Surface Monolayer of the Quantum Spin Liquid Candidate α-RuCl3. United States. https://doi.org/10.1088/2053-1583/ab7e0e
Dai, Zhongwei, Yu, Jie-Xiang, Zhou, Boyi, Tenney, Samuel, Lampen-Kelley, Paula, Yan, Jiaqiang, Mandrus, David G., Henriksen, Erik, Zang, Jiadong, Pohl, Karsten, and Sadowski, Jerzy T. Mon .
"Crystal Structure Reconstruction in the Surface Monolayer of the Quantum Spin Liquid Candidate α-RuCl3". United States. https://doi.org/10.1088/2053-1583/ab7e0e. https://www.osti.gov/servlets/purl/1604620.
@article{osti_1604620,
title = {Crystal Structure Reconstruction in the Surface Monolayer of the Quantum Spin Liquid Candidate α-RuCl3},
author = {Dai, Zhongwei and Yu, Jie-Xiang and Zhou, Boyi and Tenney, Samuel and Lampen-Kelley, Paula and Yan, Jiaqiang and Mandrus, David G. and Henriksen, Erik and Zang, Jiadong and Pohl, Karsten and Sadowski, Jerzy T.},
abstractNote = {α-RuCl3, a layered 2D material, was recently identified as a promising candidate for realizing a Kitaev quantum spin liquid. However one fundamental property, the crystal structure, has not been well resolved yet due to difficulty of bulk diffraction techniques caused by layer stacking faults. Furthermore, the surface relaxation of monolayer-level thin films is completely unknown yet. In this report, surface sensitive low energy electron diffraction technique with µm selectivity (µ-LEED) combined with dynamical LEED analysis were used to reveal the detailed crystal structure of the surface monolayer of α-RuCl3. A surface structural distortion that breaks the inversion symmetry of the ideal bulk structure was revealed. To be specific, we found the surface Cl sub-lattice is buckled with one Cl atom approximately 0.16 Å below the other two Cl atoms, in the unit cell. The Ru atomic layer shows an even larger buckling of approximately 0.31 Å. Through density functional theory (DFT) calculations, we suggested that this surface distortion may be induced by Cl-vacancies that are inevitable in this material system. Inversion symmetry breaking in this material could have a significant impact on the 2D Kitaev interaction for both, interfaces with other 2D materials, such as graphene and future monolayer devices.},
doi = {10.1088/2053-1583/ab7e0e},
journal = {2D Materials},
number = 3,
volume = 7,
place = {United States},
year = {Mon Mar 09 00:00:00 EDT 2020},
month = {Mon Mar 09 00:00:00 EDT 2020}
}
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