Interlayer coupling and gate-tunable excitons in transition metal dichalcogenide heterostructures

Abstract

Bilayer van der Waals (vdW) heterostructures such as MoS2/WS2 and MoSe2/WSe2 have attracted much attention recently, particularly because of their type II band alignments and the formation of interlayer exciton as the lowest-energy excitonic state. In this work, we calculate the electronic and optical properties of such heterostructures with the first-principles GW+Bethe-Salpeter Equation (BSE) method and reveal the important role of interlayer coupling in deciding the excited-state properties, including the band alignment and excitonic properties. Our calculation shows that due to the interlayer coupling, the low energy excitons can be widely tunable by a vertical gate field. In particular, the dipole oscillator strength and radiative lifetime of the lowest energy exciton in these bilayer heterostructures is varied by over an order of magnitude within a practical external gate field. We also build a simple model that captures the essential physics behind this tunability and allows the extension of the ab initio results to a large range of electric fields. Our work clarifies the physical picture of interlayer excitons in bilayer vdW heterostructures and predicts a wide range of gate-tunable excited-state properties of 2D optoelectronic devices.

16 pages with 4 figures and 1 table

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• Theory of Coulomb Drag in Spatially Inhomogeneous Materials
• Valley Degree of Freedom in Two-Dimensional van der Waals Materials
• Anisotropic Electron-Hole Excitation and Large Linear Dichroism in Two-Dimensional Ferromagnet CrSBr with In-Plane Magnetization
• Oxygen-induced in-situ manipulation of the interlayer coupling and exciton recombination in Bi2Se3/MoS2 2D heterostructures
• Interlayer Exciton Valleytronics in Bilayer Heterostructures Interfaced with a Metasurface
• Anomalous exciton transport in response to a uniform, in-plane electric field
• Quantum Geometric Exciton Drift Velocity
• Intrinsic control of interlayer exciton generation rate in van der Waals materials via Janus layers
• Theoretical investigation of the vertical dielectric screening dependence on defects for few-layered van der Waals materials
• Dielectric screening at TMD:hBN interfaces: Monolayer-to-bulk transition, local-field effect, and spatial dependence
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• Electrical control of orbital and vibrational interlayer coupling in bi- and trilayer 2H-MoS${}_2$
• Electrically tunable MoSe${}_2$/WSe${}_2$ heterostructure-based quantum dot
• Modulating Peierls distortion of 1T_prime MoS2 via charge doping: a new charge density wave phase, reversible phase transition, and excellent electromechanical properties
• Enhancement of the WS${}_2$ A${}_{1\text{g}}$ Raman Mode in MoS${}_2$/WS${}_2$ Heterostructures
• Interlayer Coupling Effect in van der Waals Heterostructures of Transition Metal Dichalcogenides
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