Density Functional Theory for 2D Transition-Metal Dichalcogenides with Extended Hubbard Parameters
Abstract
Accurate modelling of the band-edge electronic structure of transition metal dichalcogenides (TMDs), such as MoS2, is essential for understanding their optical, electronic and spintronic properties and enabling future applications. Here, we supplement the standard PBE exchange-correlation functional with on-metal (U) and metal--chalcogen (V) Hubbard corrections, which can control the orbital composition of band-edge states and consequently improve the quantitative accuracy of various properties. For MoS2, MoSe2, WS2, and WSe2, we optimise the U and V parameters by comparison with experimentally measured spin--orbit splittings at the conduction and valence band edges, and show that these optimal choices also improve agreement of the computed band gap, and ferroelectric potential drop in rhombohedral bilayers, with experimentally measured values. This provides a highly efficient, scalable framework for quantitatively accurate, high-throughput calculations of monolayer and multilayer TMDs, suitable for implementation in 2D-materials databases, as well as large-scale electronic and spintronic device modelling.
Related
- Interplay of Excitonic Charge Density Wave and Superconductivity in Transition Metal Dichalcogenides
- Photogalvanic effect in monolayers of transition metal dichalcogenides
- Doping-driven Mott transition from steady-state density functional theory
- Higher order anharmonicity and polymorphism in the lattice thermal conductivity of transition metal dichalcogenides
- Ab initio exploration of hydrogen-intercalated transition metal dichalcogenides: From identifying stable structures to emergent superconductivity
BibTeX
@misc{li2026density,
title = {{Density Functional Theory for 2D Transition-Metal Dichalcogenides with Extended Hubbard Parameters}},
author = {Xue Li and Suad Alshammari and Igor Rozhansky and James G. McHugh and Vladimir Fal'ko},
howpublished = {arXiv},
year = {2026},
month = oct,
doi = {10.48550/arxiv.2610.05496},
eprint = {2610.05496},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2610.05496},
}
RIS
TY - UNPB
TI - Density Functional Theory for 2D Transition-Metal Dichalcogenides with Extended Hubbard Parameters
AU - Xue Li
AU - Suad Alshammari
AU - Igor Rozhansky
AU - James G. McHugh
AU - Vladimir Fal'ko
PY - 2026
DA - 2026/10/12
PB - arXiv
DO - 10.48550/arxiv.2610.05496
UR - https://arxiv.org/abs/2610.05496
AB - Accurate modelling of the band-edge electronic structure of transition metal dichalcogenides (TMDs), such as MoS_2, is essential for understanding their optical, electronic and spintronic properties and enabling future applications. Here, we supplement the standard PBE exchange-correlation functional with on-metal (U) and metal--chalcogen (V) Hubbard corrections, which can control the orbital composition of band-edge states and consequently improve the quantitative accuracy of various properties. For MoS_2, MoSe_2, WS_2, and WSe_2, we optimise the U and V parameters by comparison with experimentally measured spin--orbit splittings at the conduction and valence band edges, and show that these optimal choices also improve agreement of the computed band gap, and ferroelectric potential drop in rhombohedral bilayers, with experimentally measured values. This provides a highly efficient, scalable framework for quantitatively accurate, high-throughput calculations of monolayer and multilayer TMDs, suitable for implementation in 2D-materials databases, as well as large-scale electronic and spintronic device modelling.
ER -