Accurate force-field methodology capturing atomic reconstructions in transition metal dichalcogenide moiré systems

Abstract

In this work, a generalized force-field methodology for the relaxation of large moiré heterostructures is proposed. The force-field parameters are optimized to accurately reproduce the structural degrees of freedom of some computationally manageable cells relaxed using density functional theory. The parameters can then be used to handle large moiré systems. We specialize to the case of 2H-phased twisted transition-metal dichalcogenide homo- and heterobilayers using a combination of the Stillinger-Weber intralayer- and the Kolmogorov-Crespi interlayer-potential. Force-field parameters are developed for all combinations of MX${}_2$ for $\text{M}\in \{\text{Mo},\text{W}\}$ and $\text{X}\in \{\text{S},\text{Se},\text{Te}\}$. The results show agreement within 20 meV in terms of band structure between density functional theory and force-field relaxation. Using the relaxed structures, a simplified and systematic scheme for the extraction of the interlayer moiré potential is presented for both R- and H-stacked systems. We show that in-plane and out-of-plane relaxation effects on the moiré potential, which is made both deeper and wider after relaxation, are essential. An interpolation based methodology for the calculation of the interlayer binding energy is also proposed. Finally, we show that atomic reconstruction, which is captured by the force-field method, becomes especially prominent for angles below 4-5${}^{\circ }$, when there is no mismatch in lattice constant between layers.

arXiv comment11 pages, 12 figures. Accepted by and to be published in Physical Review B

References in corpus (40)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Advanced capabilities for materials modelling with Quantum ESPRESSO
• 2D materials and van der Waals heterostructures
• Optimized norm-conserving Vanderbilt pseudopotentials
• Moire bands in twisted double-layer graphene
• The PseudoDojo: Training and grading a 85 element optimized norm-conserving pseudopotential table
• Magnetic 2D materials and heterostructures
• Moiré Excitons in Van der Waals Heterostructures
• Optical detection of Mott and generalized Wigner crystal states in WSe2/WS2 moiré superlattices
• Quasiparticle band structures and optical properties of strained monolayer MoS2 and WS2
• Topological insulators in twisted transition metal dichalcogenide homobilayers
• Hubbard model physics in transition metal dichalcogenide moiré bands
• Moiré excitons: from programmable quantum emitter arrays to spin-orbit coupled artificial lattices
• Band Alignment of 2D Semiconductors for Designing Heterostructures with Momentum Space Matching
• Ultraflat bands and shear solitons in Moiré patterns of twisted bilayer transition metal dichalcogenides
• Atomic reconstruction in twisted bilayers of transition metal dichalcogenides
• Topological Exciton Bands in Moiré Heterojunctions
• Theory of optical absorption by interlayer excitons in transition metal dichalcogenide heterobilayers
• Relaxation and Domain Formation in Incommensurate 2D Heterostructures
• Atomic reconstruction and moiré patterns in transition metal dichalcogenide van der Waals heterostructures
• Deep moiré potentials in twisted transition metal dichalcogenide bilayers
• Imaging moiré flat bands in 3D reconstructed WSe2/WS2 superlattices
• Stacking domains and dislocation networks in marginally twisted bilayers of transition metal dichalcogenides
• Nanoserpents: Graphene Nanoribbons Motion on Two-Dimensional Hexagonal Materials
• Band topology, Hubbard model, Heisenberg model, and Dzyaloshinskii-Moriya interaction in twisted bilayer WSe${}_2$
• Broken mirror symmetry in excitonic response of reconstructed domains in twisted MoSe${}_2$/MoSe${}_2$ bilayers
• Tunable Phases of Moiré Excitons in van der Waals Heterostructures
• Moiré Potential Impedes Interlayer Exciton Diffusion in van der Waals Heterostructures
• Quantum Phase Diagram of a Moiré-Hubbard Model
• Inter-layer Potential for Hexagonal Boron Nitride
• Moiré metrology of energy landscapes in van der Waals heterostructures
• Shedding Light on Moire Excitons: A First-Principles Perspective
• Charge Transfer Excitations, Pair Density Waves, and Superconductivity in Moiré Materials
• Spin-Orbit Coupling in Transition Metal Dichalcogenide Heterobilayer Flat Bands
• Moiré-Bose-Hubbard model for interlayer excitons in twisted transition metal dichalcogenide heterostructures
• Theory of tunable flux lattices in the homobilayer moiré of twisted and uniformly strained transition metal dichalcogenides
• Reconstruction of moiré lattices in twisted transition metal dichalcogenide bilayers
• Key role of the moire potential for the quasi-condensation of interlayer excitons in van der Waals heterostructures
• Twist versus heterostrain control of optical properties of moiré exciton minibands
• Noncollinear topological textures in two-dimensional van der Waals materials: From magnetic to polar systems

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• Laterally Extended States of Interlayer Excitons in Reconstructed MoSe${}_2$/WSe${}_2$ Heterostructures
• Effective long-range attraction of moiré excitons under the influence of atomic reconstructions and anisotropic screening