Theoretical study of the crystal and electronic properties of α - RuI 3
Abstract
The material α-RuCl3, with a two-dimensional Ru honeycomb sublattice, has attracted considerable attention because it may be a realization of the Kitaev quantum spin liquid. Recently, a new honeycomb material, α-RuCl3, was prepared under moderately high pressure, and it is stable under ambient conditions. However, different from α-RuCl3, α-RuI3 was reported to be a paramagnetic metal without long-range magnetic order down to 0.35 K. Here, the structural and electronic properties of the quasi-two-dimensional α-RuI3 are theoretically studied. First, based on first-principles density functional theory calculations, the ABC stacking honeycomb-layer R$$\bar{3}$$ (No. 148) structure is found to be the most likely stacking order for α-RuI3 along the c axis. Furthermore, both R$$\bar{3}$$ and P$$\bar{3}$$1c are dynamically stable because no imaginary frequency modes were obtained in the phononic dispersion spectrum without Hubbard U. Moreover, the different physical behavior of α-RuI3 compared to α-RuCl3 can be understood naturally. The strong hybridization between Ru 4d and I 5p orbitals decreases the “effective” atomic Hubbard repulsion, leading the electrons of RuI3 to be less localized than in RuCl3. As a consequence, the effective electronic correlation is reduced from Cl to I, leading to the metallic nature of α-RuI3. Based on the DFT+U (Ueff=2 eV) plus spin-orbital coupling, we obtained a spin-orbit Mott insulating behavior for α-RuCl3 and, with the same procedure, a metallic behavior for α-RuI3, in good agreement with experimental results. Furthermore, when introducing large (unrealistic) Ueff=6 eV, the spin-orbit Mott gap opens in α-RuI3 as well, supporting the physical picture we are proposing. Our results provide guidance to experimentalists and theorists working on two-dimensional transition metal tri-iodide layered materials.
- Authors:
-
- Univ. of Tennessee, Knoxville, TN (United States)
- Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
- OSTI Identifier:
- 1870232
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review. B
- Additional Journal Information:
- Journal Volume: 105; Journal Issue: 8; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; electronic structure; 2-dimensional systems; honeycomb lattice; strongly correlated systems; density functional calculations; first-principles calculations
Citation Formats
Zhang, Yang, Lin, Ling-Fang, Moreo, Adriana, and Dagotto, Elbio. Theoretical study of the crystal and electronic properties of α-RuI3. United States: N. p., 2022.
Web. doi:10.1103/physrevb.105.085107.
Zhang, Yang, Lin, Ling-Fang, Moreo, Adriana, & Dagotto, Elbio. Theoretical study of the crystal and electronic properties of α-RuI3. United States. https://doi.org/10.1103/physrevb.105.085107
Zhang, Yang, Lin, Ling-Fang, Moreo, Adriana, and Dagotto, Elbio. Fri .
"Theoretical study of the crystal and electronic properties of α-RuI3". United States. https://doi.org/10.1103/physrevb.105.085107. https://www.osti.gov/servlets/purl/1870232.
@article{osti_1870232,
title = {Theoretical study of the crystal and electronic properties of α-RuI3},
author = {Zhang, Yang and Lin, Ling-Fang and Moreo, Adriana and Dagotto, Elbio},
abstractNote = {The material α-RuCl3, with a two-dimensional Ru honeycomb sublattice, has attracted considerable attention because it may be a realization of the Kitaev quantum spin liquid. Recently, a new honeycomb material, α-RuCl3, was prepared under moderately high pressure, and it is stable under ambient conditions. However, different from α-RuCl3, α-RuI3 was reported to be a paramagnetic metal without long-range magnetic order down to 0.35 K. Here, the structural and electronic properties of the quasi-two-dimensional α-RuI3 are theoretically studied. First, based on first-principles density functional theory calculations, the ABC stacking honeycomb-layer R$\bar{3}$ (No. 148) structure is found to be the most likely stacking order for α-RuI3 along the c axis. Furthermore, both R$\bar{3}$ and P$\bar{3}$1c are dynamically stable because no imaginary frequency modes were obtained in the phononic dispersion spectrum without Hubbard U. Moreover, the different physical behavior of α-RuI3 compared to α-RuCl3 can be understood naturally. The strong hybridization between Ru 4d and I 5p orbitals decreases the “effective” atomic Hubbard repulsion, leading the electrons of RuI3 to be less localized than in RuCl3. As a consequence, the effective electronic correlation is reduced from Cl to I, leading to the metallic nature of α-RuI3. Based on the DFT+U (Ueff=2 eV) plus spin-orbital coupling, we obtained a spin-orbit Mott insulating behavior for α-RuCl3 and, with the same procedure, a metallic behavior for α-RuI3, in good agreement with experimental results. Furthermore, when introducing large (unrealistic) Ueff=6 eV, the spin-orbit Mott gap opens in α-RuI3 as well, supporting the physical picture we are proposing. Our results provide guidance to experimentalists and theorists working on two-dimensional transition metal tri-iodide layered materials.},
doi = {10.1103/physrevb.105.085107},
journal = {Physical Review. B},
number = 8,
volume = 105,
place = {United States},
year = {Fri Feb 04 00:00:00 EST 2022},
month = {Fri Feb 04 00:00:00 EST 2022}
}
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