Computational Analysis of Interface-Driven Spin-Orbit Coupling in Molecular Adsorbates on Transition Metal Dichalcogenides

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Auteurs principaux: Wang, Zihao, Li, Wan-Lu, Li, Shaowei
Format: Preprint
Publié: 2025
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author Wang, Zihao
Li, Wan-Lu
Li, Shaowei
author_facet Wang, Zihao
Li, Wan-Lu
Li, Shaowei
contents Spin-orbit coupling (SOC) lifts molecular orbital degeneracy, enabling bi-level electronic platforms suitable for next-generation digital devices. However, common light-atom molecular feedstocks exhibit weak SOC due to the absence of heavy elements. To enhance SOC without synthesizing new materials, we leverage interfacial interactions between molecules and transition-element-based solid-state materials. This computational study investigates SOC splitting in metal-phthalocyanine adsorbed on transition metal dichalcogenides (TMDs) using density functional theory (DFT). The enhanced SOC splitting is attributed to strong orbital hybridization at the molecule-substrate interface. Specifically, Zn-phthalocyanine (ZnPC) on monolayer MoS2 achieves a notable SOC splitting of ~8 meV. Furthermore, when ZnPC forms self-assembled chains on MoS2, the splitting increases to ~20 meV, driven by the formation of hybrid bands modulated by molecular periodicity. These findings highlight the role of interfacial and intermolecular interactions in inducing and enhancing SOC in surface-adsorbed molecules, providing a new strategy for molecular spintronic materials without complex synthetic efforts.
format Preprint
id arxiv_https___arxiv_org_abs_2505_03187
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Computational Analysis of Interface-Driven Spin-Orbit Coupling in Molecular Adsorbates on Transition Metal Dichalcogenides
Wang, Zihao
Li, Wan-Lu
Li, Shaowei
Materials Science
Chemical Physics
Computational Physics
Spin-orbit coupling (SOC) lifts molecular orbital degeneracy, enabling bi-level electronic platforms suitable for next-generation digital devices. However, common light-atom molecular feedstocks exhibit weak SOC due to the absence of heavy elements. To enhance SOC without synthesizing new materials, we leverage interfacial interactions between molecules and transition-element-based solid-state materials. This computational study investigates SOC splitting in metal-phthalocyanine adsorbed on transition metal dichalcogenides (TMDs) using density functional theory (DFT). The enhanced SOC splitting is attributed to strong orbital hybridization at the molecule-substrate interface. Specifically, Zn-phthalocyanine (ZnPC) on monolayer MoS2 achieves a notable SOC splitting of ~8 meV. Furthermore, when ZnPC forms self-assembled chains on MoS2, the splitting increases to ~20 meV, driven by the formation of hybrid bands modulated by molecular periodicity. These findings highlight the role of interfacial and intermolecular interactions in inducing and enhancing SOC in surface-adsorbed molecules, providing a new strategy for molecular spintronic materials without complex synthetic efforts.
title Computational Analysis of Interface-Driven Spin-Orbit Coupling in Molecular Adsorbates on Transition Metal Dichalcogenides
topic Materials Science
Chemical Physics
Computational Physics
url https://arxiv.org/abs/2505.03187