Crystal Structure Reconstruction in the Surface Monolayer of the Quantum Spin Liquid Candidate α-RuCl3

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.

doi:10.1088/2053-1583/ab7e0e

Title: Crystal Structure Reconstruction in the Surface Monolayer of the Quantum Spin Liquid Candidate α-RuCl₃

Journal Article · Mon Mar 09 00:00:00 EDT 2020 · 2D Materials

DOI:https://doi.org/10.1088/2053-1583/ab7e0e· OSTI ID:1604620

^[1]; Yu, Jie-Xiang ^[2]; Zhou, Boyi ^[3]; Tenney, Samuel ^[1]; Lampen-Kelley, Paula ^[4];

^[4]; Mandrus, David G. ^[4]; Henriksen, Erik ^[3]; Zang, Jiadong ^[5]; Pohl, Karsten ^[5];

^[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)

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.

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Research Organization:: 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 Organization:: 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)

Grant/Contract Number:: SC0012704; TG-PHY170023; PHY-1229408; GBMF4416; AC05-00OR22725

OSTI ID:: 1604620

Alternate ID(s):: OSTI ID: 1649057

Report Number(s):: BNL-213716-2020-JAAM

Journal Information:: 2D Materials, Vol. 7, Issue 3; ISSN 2053-1583

Publisher:: IOP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 8 works

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