Deriving models for the Kitaev spinliquid candidate material $\alpha \text{}{\mathrm{RuCl}}_{3}$ from first principles
Abstract
We use the constrained random phase approximation to derive from first principles the Ru$$t_{2_g}$$ Wannierfunctionbased model for the Kitaev spinliquid candidate material $α$RuCl_{3}. We find the nonlocal Coulomb repulsion to be sizable compared to the local one. In addition we obtain the contribution to the Hamiltonian from the spinorbit coupling and find it to also contain nonnegligible nonlocal terms. We invoke strongcoupling perturbation theory to investigate the influence of these nonlocal elements of the Coulomb repulsion and the spinorbit coupling on the magnetic interactions. We find that the nonlocal Coulomb repulsions cause a strong enhancement of the magnetic interactions, which deviate from experimental fits reported in the literature. Our results contribute to the understanding and design of quantum spinliquid materials via firstprinciples calculations.
 Authors:

 Univ. of Tennessee, Knoxville, TN (United States)
 Louisiana State Univ., Baton Rouge, LA (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
 OSTI Identifier:
 1566977
 Alternate Identifier(s):
 OSTI ID: 1547988
 Grant/Contract Number:
 AC0500OR22725
 Resource Type:
 Accepted Manuscript
 Journal Name:
 Physical Review B
 Additional Journal Information:
 Journal Volume: 100; Journal Issue: 7; Journal ID: ISSN 24699950
 Publisher:
 American Physical Society (APS)
 Country of Publication:
 United States
 Language:
 English
 Subject:
 36 MATERIALS SCIENCE
Citation Formats
Eichstaedt, Casey, Zhang, Yi, Laurell, Pontus Bengt Johan, Okamoto, Satoshi, Eguiluz, Adolfo, and Berlijn, Tom. Deriving models for the Kitaev spinliquid candidate material αRuCl3 from first principles. United States: N. p., 2019.
Web. doi:10.1103/PhysRevB.100.075110.
Eichstaedt, Casey, Zhang, Yi, Laurell, Pontus Bengt Johan, Okamoto, Satoshi, Eguiluz, Adolfo, & Berlijn, Tom. Deriving models for the Kitaev spinliquid candidate material αRuCl3 from first principles. United States. doi:10.1103/PhysRevB.100.075110.
Eichstaedt, Casey, Zhang, Yi, Laurell, Pontus Bengt Johan, Okamoto, Satoshi, Eguiluz, Adolfo, and Berlijn, Tom. Tue .
"Deriving models for the Kitaev spinliquid candidate material αRuCl3 from first principles". United States. doi:10.1103/PhysRevB.100.075110. https://www.osti.gov/servlets/purl/1566977.
@article{osti_1566977,
title = {Deriving models for the Kitaev spinliquid candidate material αRuCl3 from first principles},
author = {Eichstaedt, Casey and Zhang, Yi and Laurell, Pontus Bengt Johan and Okamoto, Satoshi and Eguiluz, Adolfo and Berlijn, Tom},
abstractNote = {We use the constrained random phase approximation to derive from first principles the Ru$t_{2_g}$ Wannierfunctionbased model for the Kitaev spinliquid candidate material $α$RuCl3. We find the nonlocal Coulomb repulsion to be sizable compared to the local one. In addition we obtain the contribution to the Hamiltonian from the spinorbit coupling and find it to also contain nonnegligible nonlocal terms. We invoke strongcoupling perturbation theory to investigate the influence of these nonlocal elements of the Coulomb repulsion and the spinorbit coupling on the magnetic interactions. We find that the nonlocal Coulomb repulsions cause a strong enhancement of the magnetic interactions, which deviate from experimental fits reported in the literature. Our results contribute to the understanding and design of quantum spinliquid materials via firstprinciples calculations.},
doi = {10.1103/PhysRevB.100.075110},
journal = {Physical Review B},
number = 7,
volume = 100,
place = {United States},
year = {2019},
month = {8}
}
Web of Science
Works referenced in this record:
Breakdown of magnons in a strongly spinorbital coupled magnet
journal, October 2017
 Winter, Stephen M.; Riedl, Kira; Maksimov, Pavel A.
 Nature Communications, Vol. 8, Issue 1
Generalized Gradient Approximation Made Simple
journal, October 1996
 Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
 Physical Review Letters, Vol. 77, Issue 18, p. 38653868
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
Anyons in an exactly solved model and beyond
journal, January 2006
 Kitaev, Alexei
 Annals of Physics, Vol. 321, Issue 1
Monoclinic crystal structure of $\alpha {\mathrm{RuCl}}_{3}$ 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
Anisotropic susceptibilities in the honeycomb Kitaev system $\alpha {\mathrm{RuCl}}_{3}$
journal, September 2018
 LampenKelley, P.; Rachel, S.; Reuther, J.
 Physical Review B, Vol. 98, Issue 10
High antiferromagnetic transition temperature of the honeycomb compound ${\mathrm{SrRu}}_{2}{\mathrm{O}}_{6}$
journal, September 2015
 Tian, W.; Svoboda, C.; Ochi, M.
 Physical Review B, Vol. 92, Issue 10
Challenges in design of Kitaev materials: Magnetic interactions from competing energy scales
journal, June 2016
 Winter, Stephen M.; Li, Ying; Jeschke, Harald O.
 Physical Review B, Vol. 93, Issue 21
Unusual Thermal Hall Effect in a Kitaev Spin Liquid Candidate $\alpha \text{\u2212}{\mathrm{RuCl}}_{3}$
journal, May 2018
 Kasahara, Y.; Sugii, K.; Ohnishi, T.
 Physical Review Letters, Vol. 120, Issue 21
Magnetic order in $\alpha {\text{RuCl}}_{3}$ : A honeycomblattice quantum magnet with strong spinorbit coupling
journal, April 2015
 Sears, J. A.; Songvilay, M.; Plumb, K. W.
 Physical Review B, Vol. 91, Issue 14
Excitations in the fieldinduced quantum spin liquid state of αRuCl3
journal, February 2018
 Banerjee, Arnab; LampenKelley, Paula; Knolle, Johannes
 npj Quantum Materials, Vol. 3, Issue 1
Spinorbit coupling in an $f$ electron tightbinding model: Electronic properties of Th, U, and Pu
journal, January 2009
 Jones, M. D.; Albers, R. C.
 Physical Review B, Vol. 79, Issue 4
Full orbital calculation scheme for materials with strongly correlated electrons
journal, March 2005
 Anisimov, V. I.; Kondakov, D. E.; Kozhevnikov, A. V.
 Physical Review B, Vol. 71, Issue 12
Insulating Ferromagnetism in ${\mathrm{L}\mathrm{a}}_{4}{\mathrm{B}\mathrm{a}}_{2}{\mathrm{C}\mathrm{u}}_{2}{\mathrm{O}}_{10}$ : An Ab Initio Wannier Function Analysis
journal, September 2002
 Ku, Wei; Rosner, H.; Pickett, W. E.
 Physical Review Letters, Vol. 89, Issue 16
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
Majorana quantization and halfinteger thermal quantum Hall effect in a Kitaev spin liquid
journal, July 2018
 Kasahara, Y.; Ohnishi, T.; Mizukami, Y.
 Nature, Vol. 559, Issue 7713
Comparison of Ab initio LowEnergy Models for LaFePO, LaFeAsO, BaFe _{2} As _{2} , LiFeAs, FeSe, and FeTe: Electron Correlation and Covalency
journal, April 2010
 Miyake, Takashi; Nakamura, Kazuma; Arita, Ryotaro
 Journal of the Physical Society of Japan, Vol. 79, Issue 4
Spin Waves and Revised Crystal Structure of Honeycomb Iridate ${\mathrm{Na}}_{2}{\mathrm{IrO}}_{3}$
journal, March 2012
 Choi, S. K.; Coldea, R.; Kolmogorov, A. N.
 Physical Review Letters, Vol. 108, Issue 12
On Löwdin's method of symmetric orthogonalization*: Löwdin's Method of Symmetric Orthogonalization
journal, January 2002
 Mayer, I.
 International Journal of Quantum Chemistry, Vol. 90, Issue 1
Maximally localized generalized Wannier functions for composite energy bands
journal, November 1997
 Marzari, Nicola; Vanderbilt, David
 Physical Review B, Vol. 56, Issue 20
Majorana fermions in the Kitaev quantum spin system αRuCl3
journal, September 2017
 Do, SeungHwan; Park, SangYoun; Yoshitake, Junki
 Nature Physics, Vol. 13, Issue 11
Kitaev magnetism in honeycomb ${\text{RuCl}}_{3}$ with intermediate spinorbit coupling
journal, June 2015
 Kim, HeungSik; V., Vijay Shankar; Catuneanu, Andrei
 Physical Review B, Vol. 91, Issue 24
Successive magnetic phase transitions in $\alpha {\mathrm{RuCl}}_{3}$ : XYlike frustrated magnet on the honeycomb lattice
journal, March 2015
 Kubota, Yumi; Tanaka, Hidekazu; Ono, Toshio
 Physical Review B, Vol. 91, Issue 9
Effective Hamiltonian for cuprate superconductors derived from multiscale ab initio scheme with level renormalization
journal, June 2019
 Hirayama, Motoaki; Misawa, Takahiro; Ohgoe, Takahiro
 Physical Review B, Vol. 99, Issue 24
KitaevHeisenberg ${J}_{2}$  ${J}_{3}$ model for the iridates ${A}_{2}$ IrO ${}_{3}$
journal, November 2011
 Kimchi, Itamar; You, YiZhuang
 Physical Review B, Vol. 84, Issue 18
Spinwave analysis of the lowtemperature thermal Hall effect in the candidate Kitaev spin liquid $\alpha {\mathrm{RuCl}}_{3}$
journal, August 2018
 Cookmeyer, Jonathan; Moore, Joel E.
 Physical Review B, Vol. 98, Issue 6
Ab initio Studies on the Interplay between SpinOrbit Interaction and Coulomb Correlation in ${\mathrm{Sr}}_{2}{\mathrm{IrO}}_{4}$ and ${\mathrm{Ba}}_{2}{\mathrm{IrO}}_{4}$
journal, February 2012
 Arita, R.; Kuneš, J.; Kozhevnikov, A. V.
 Physical Review Letters, Vol. 108, Issue 8
NonAbelian anyons and topological quantum computation
journal, September 2008
 Nayak, Chetan; Simon, Steven H.; Stern, Ady
 Reviews of Modern Physics, Vol. 80, Issue 3
$\alpha {\mathrm{RuCl}}_{3}$ : A spinorbit 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
Unveiling magnetic interactions of ruthenium trichloride via constraining direction of orbital moments: Potential routes to realize a quantum spin liquid
journal, August 2017
 Hou, Y. S.; Xiang, H. J.; Gong, X. G.
 Physical Review B, Vol. 96, Issue 5
Faulttolerant quantum computation by anyons
journal, January 2003
 Kitaev, A. Yu.
 Annals of Physics, Vol. 303, Issue 1
Direct evidence of a zigzag spinchain structure in the honeycomb lattice: A neutron and xray diffraction investigation of singlecrystal Na ${}_{2}$ IrO ${}_{3}$
journal, May 2012
 Ye, Feng; Chi, Songxue; Cao, Huibo
 Physical Review B, Vol. 85, Issue 18
Limitations of constrained random phase approximation downfolding
journal, December 2018
 Honerkamp, Carsten; Shinaoka, Hiroshi; Assaad, Fakher F.
 Physical Review B, Vol. 98, Issue 23
Derivation of static lowenergy effective models by an ab initio downfolding method without double counting of Coulomb correlations: Application to SrVO ${}_{3}$ , FeSe, and FeTe
journal, May 2013
 Hirayama, Motoaki; Miyake, Takashi; Imada, Masatoshi
 Physical Review B, Vol. 87, Issue 19
Kitaev exchange and fieldinduced quantum spinliquid states in honeycomb αRuCl3
journal, November 2016
 Yadav, Ravi; Bogdanov, Nikolay A.; Katukuri, Vamshi M.
 Scientific Reports, Vol. 6, Issue 1
KitaevHeisenberg Model on a Honeycomb Lattice: Possible Exotic Phases in Iridium Oxides ${A}_{2}{\mathrm{IrO}}_{3}$
journal, July 2010
 Chaloupka, Jiří; Jackeli, George; Khaliullin, Giniyat
 Physical Review Letters, Vol. 105, Issue 2
Crystal structure and magnetism in $\alpha {\mathrm{RuCl}}_{3}$ : An ab initio study
journal, April 2016
 Kim, HeungSik; Kee, HaeYoung
 Physical Review B, Vol. 93, Issue 15
Field evolution of magnons in $\alpha \text{\u2212}{\mathrm{RuCl}}_{3}$ by highresolution polarized terahertz spectroscopy
journal, September 2018
 Wu, Liang; Little, A.; Aldape, E. E.
 Physical Review B, Vol. 98, Issue 9
Mott Insulators in the Strong SpinOrbit 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
${\mathrm{Na}}_{2}{\mathrm{IrO}}_{3}$ as a Molecular Orbital Crystal
journal, November 2012
 Mazin, I. I.; Jeschke, Harald O.; Foyevtsova, Kateryna
 Physical Review Letters, Vol. 109, Issue 19
Longrange magnetic ordering in Na ${}_{2}$ IrO ${}_{3}$
journal, June 2011
 Liu, X.; Berlijn, T.; Yin, W. G.
 Physical Review B, Vol. 83, Issue 22
Ab initio derivation of an effective Hamiltonian for the ${\mathrm{La}}_{2}{\mathrm{CuO}}_{4}/{\mathrm{La}}_{1.55}{\mathrm{Sr}}_{0.45}{\mathrm{CuO}}_{4}$ heterostructure
journal, April 2019
 Tadano, Terumasa; Nomura, Yusuke; Imada, Masatoshi
 Physical Review B, Vol. 99, Issue 15
Effective model with strong Kitaev interactions for $\alpha \text{\u2212}{\mathrm{RuCl}}_{3}$
journal, April 2018
 Suzuki, Takafumi; Suga, Seiichiro
 Physical Review B, Vol. 97, Issue 13
SpinWave Excitations Evidencing the Kitaev Interaction in Single Crystalline $\alpha \text{\u2212}{\mathrm{RuCl}}_{3}$
journal, March 2017
 Ran, Kejing; Wang, Jinghui; Wang, Wei
 Physical Review Letters, Vol. 118, Issue 10
FirstPrinciples Study of the HoneycombLattice Iridates ${\mathrm{Na}}_{2}{\mathrm{IrO}}_{3}$ in the Presence of Strong SpinOrbit Interaction and Electron Correlations
journal, September 2014
 Yamaji, Youhei; Nomura, Yusuke; Kurita, Moyuru
 Physical Review Letters, Vol. 113, Issue 10
Theoretical investigation of magnetic dynamics in $\alpha {\mathrm{RuCl}}_{3}$
journal, September 2017
 Wang, Wei; Dong, ZhaoYang; Yu, ShunLi
 Physical Review B, Vol. 96, Issue 11
Lowtemperature crystal and magnetic structure of $\alpha {\mathrm{RuCl}}_{3}$
journal, April 2016
 Cao, H. B.; Banerjee, A.; Yan, J. Q.
 Physical Review B, Vol. 93, Issue 13
Works referencing / citing this record:
Dynamical and thermal magnetic properties of the Kitaev spin liquid candidate αRuCl3
journal, January 2020
 Laurell, Pontus; Okamoto, Satoshi
 npj Quantum Materials, Vol. 5, Issue 1