Giant proximity exchange and valley splitting in transition metal dichalcogenide/$h\mathrm{BN}$/(Co, Ni) heterostructures

TL;DR

This study reveals significant proximity-induced exchange effects and valley splitting in TMDC/hBN/FM heterostructures, with large exciton peak splittings driven by hybridization with ferromagnetic metals, useful for spintronic applications.

Contribution

First-principles analysis of proximity exchange and valley splitting in TMDC/hBN/FM heterostructures, introducing a minimal tight-binding model to quantify exchange parameters and exciton effects.

Findings

Proximity exchange parameters range from 1 to 10 meV depending on the ferromagnet.

Giant exciton peak splittings up to 8 meV in MoS₂/hBN/Co structures.

Band hybridization with Co d orbitals causes large valence band exchange splitting.

Abstract

We investigate the proximity-induced exchange coupling in transition-metal dichalcogenides (TMDCs), originating from spin injector geometries composed of hexagonal boron-nitride (hBN) and ferromagnetic (FM) cobalt (Co) or nickel (Ni), from first-principles. We employ a minimal tight-binding Hamiltonian that captures the low energy bands of the TMDCs around K and K' valleys, to extract orbital, spin-orbit, and exchange parameters. The TMDC/hBN/FM heterostructure calculations show that due to the hBN buffer layer, the band structure of the TMDC is preserved, with an additional proximity-induced exchange splitting in the bands. We extract proximity exchange parameters in the 1--10 meV range, depending on the FM. The combination of proximity-induced exchange and intrinsic spin-orbit coupling (SOC) of the TMDCs, leads to a valley polarization, translating into magnetic exchange fields of tens of Tesla. The extracted parameters are useful for subsequent exciton calculations of TMDCs in the presence of a hBN/FM spin injector. Our calculated absorption spectra show large splittings for the exciton peaks; in the case of MoS$_2$/hBN/Co we find a value of about 8 meV, corresponding to about 50 Tesla external magnetic field in bare TMDCs. The reason lies in the band structure, where a hybridization with Co $d$ orbitals causes a giant valence band exchange splitting of more than 10 meV. Structures with Ni do not show any $d$ level hybridization features, but still sizeable proximity exchange and exciton peak splittings of around 2 meV are present in the TMDCs.