Layer degree of freedom for excitons in transition metal dichalcogenides

Abstract

Layered transition metal dichalcogenides (TMDCs) host a variety of strongly bound exciton complexes that control the optical properties in these materials. Apart from spin and valley, layer index provides an additional degree of freedom in a few-layer thick film. Here we show that in a few-layer TMDC film, the wavefunctions of the conduction and valence band edge states contributing to the K (K') valley are spatially confined in the alternate layers - giving rise to direct (quasi-)intra-layer bright exciton and lower-energy inter-layer dark excitons. Depending on the spin and valley configuration, the bright exciton state is further found to be a coherent superposition of two layer-induced states, one (E-type) distributed in the even layers and the other (O-type) in the odd layers. The intra-layer nature of the bright exciton manifests as a relatively weak dependence of the exciton binding energy on the thickness of the few-layer film, and the binding energy is maintained up to 50 meV in the bulk limit - which is an order of magnitude higher than conventional semiconductors. Fast stokes energy transfer from the intra-layer bright state to the inter-layer dark states provides a clear signature in the layer-dependent broadening of the photoluminescence peak, and plays a key role in the suppression of the photoluminescence intensity observed in TMDCs with thickness beyond monolayer.

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• Giant optical anisotropy in transition metal dichalcogenides for next-generation photonics
• Combinatorial Large-area MoS2/Anatase-TiO2 interface: A Pathway to Emergent Optical and Opto-electronic Functionalities
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• Gate-tunable trion switch for excitonic device applications
• Electrical reversal of the sign for magnon thermal Hall coefficient in a van der Waals bilayer antiferromagnet
• Electric-field-tunable intervalley excitons and phonon replicas in bilayer WSe${}_2$
• Prediction of a layer nonlinear Hall effect in bilayer nonmagnetic or antiferromagnetic systems
• Highly tunable layered exciton in bilayer WS${}_2$: linear quantum confined Stark effect versus electrostatic doping