Electronic structure of α-RuCl3 by fixed-node and fixed-phase diffusion Monte Carlo methods

Annaberdiyev, Abdulgani; Melton, Cody A.; Wang, Guangming; Mitas, Lubos

doi:10.1103/physrevb.106.075127

Electronic structure of α- RuCl3 by fixed-node and fixed-phase diffusion Monte Carlo methods

Journal Article · Mon Aug 15 00:00:00 EDT 2022 · Physical Review. B

DOI:https://doi.org/10.1103/physrevb.106.075127· OSTI ID:1883887

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North Carolina State Univ., Raleigh, NC (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
North Carolina State Univ., Raleigh, NC (United States)

Layered material α-RuCl₃ has caught wide attention due to its possible realization of Kitaev's spin liquid and its electronic structure that involves the interplay of electron-electron correlations and spin-orbit effects. Several DFT+U studies have suggested that both electron-electron correlations and spin-orbit effects are crucial for accurately describing the band gap. This work studies the importance of these two effects using fixed-node and fixed-phase diffusion Monte Carlo calculations both in spin-averaged and explicit spin-orbit formalisms. In the latter, the Slater-Jastrow trial function is constructed from two-component spin orbitals using our recent quantum Monte Carlo (QMC) developments and thoroughly tested effective core potentials. Our results show that the gap in the ideal crystal is already accurately described by the spin-averaged case, with the dominant role being played by the magnetic ground state with significant exchange and electron correlation effects. We find qualitative agreement between hybrid DFT, DFT+U, and QMC. In addition, QMC results agree very well with available experiments, and we identify the values of exact Fock exchange mixing that provide comparable gaps. Explicit spin-orbit QMC calculations reveal that the effect of spin-orbit coupling on the gap is minor, of the order of 0.2 eV, which corresponds to the strength of the spin orbit of the Ru atom.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1883887

Alternate ID(s):: OSTI ID: 1887402

Journal Information:: Physical Review. B, Journal Name: Physical Review. B Journal Issue: 7 Vol. 106; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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