Band structures and Z2 invariants of two-dimensional transition metal dichalcogenide monolayers from fully relativistic Dirac-Kohn-Sham theory using Gaussian-type orbitals

Marius Kadek, Baokai Wang, Marc Joosten, Wei-Chi Chiu, Francois Mairesse, Michal Repisky, Kenneth Ruud, and Arun Bansil
Phys. Rev. Materials 7, 064001 – Published 2 June 2023
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Abstract

Two-dimensional (2D) materials exhibit a wide range of remarkable phenomena, many of which owe their existence to the relativistic spin-orbit coupling (SOC) effects. To understand and predict properties of materials containing heavy elements, such as the transition-metal dichalcogenides (TMDs), relativistic effects must be taken into account in first-principles calculations. We present an all-electron method based on the four-component Dirac Hamiltonian and Gaussian-type orbitals (GTOs) that overcomes complications associated with linear dependencies and ill-conditioned matrices that arise when diffuse functions are included in the basis. Until now, there has been no systematic study of the convergence of GTO basis sets for periodic solids either at the nonrelativistic or the relativistic level. Here we provide such a study of relativistic band structures of the 2D TMDs in the hexagonal (2H), tetragonal (1T), and distorted tetragonal (1T') structures, along with a discussion of their SOC-driven properties (Rashba splitting and Z2 topological invariants). We demonstrate the viability of our approach even when large basis sets with multiple basis functions involving various valence orbitals (denoted triple- and quadruple-ζ) are used in the relativistic regime. Our method does not require the use of pseudopotentials and provides access to all electronic states within the same framework. Our study paves the way for direct studies of material properties, such as the parameters in spin Hamiltonians, that depend heavily on the electron density near atomic nuclei where relativistic and SOC effects are the strongest.

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  • Received 4 March 2023
  • Accepted 19 May 2023

DOI:https://doi.org/10.1103/PhysRevMaterials.7.064001

©2023 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Marius Kadek1,2,*, Baokai Wang1, Marc Joosten2, Wei-Chi Chiu1, Francois Mairesse3, Michal Repisky2,4, Kenneth Ruud2,5, and Arun Bansil1

  • 1Department of Physics, Northeastern University, Boston, Massachusetts 02115, USA
  • 2Hylleraas Centre for Quantum Molecular Sciences, Department of Chemistry, UiT The Arctic University of Norway, N-9037 Tromsø, Norway
  • 3Laboratory of Theoretical Chemistry, University of Namur, B-5000 Namur, Belgium
  • 4Department of Physical and Theoretical Chemistry, Faculty of Natural Sciences, Comenius University, Bratislava, Slovakia
  • 5Norwegian Defence Research Establishment, P.O. Box 25, 2027 Kjeller, Norway

  • *marius.kadek@uit.no

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Issue

Vol. 7, Iss. 6 — June 2023

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