Excitonic signatures of ferroelectric order in parallel-stacked MoS${}_2$

Abstract

Interfacial ferroelectricity, prevalent in various parallel-stacked layered materials, allows switching of out-of-plane ferroelectric order by in-plane sliding of adjacent layers. Its resilience against doping potentially enables next-generation storage and logic devices. However, studies have been limited to indirect sensing or visualization of ferroelectricity. For transition metal dichalcogenides, there is little knowledge about the influence of ferroelectric order on their intrinsic valley and excitonic properties. Here, we report direct probing of ferroelectricity in few-layer 3R-MoS${}_2$ using reflectance contrast spectroscopy. Contrary to a simple electrostatic perception, layer-hybridized excitons with out-of-plane electric dipole moment remain decoupled from ferroelectric ordering, while intralayer excitons with in-plane dipole orientation are sensitive to it. Ab initio calculations identify stacking-specific interlayer hybridization leading to this asymmetric response. Exploiting this sensitivity, we demonstrate optical readout and control of multi-state polarization with hysteretic switching in a field-effect device. Time-resolved Kerr ellipticity reveals a direct correspondence between spin-valley dynamics and stacking order.

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Cited by in corpus (9)

• Roadmap for Photonics with 2D Materials
• Plasmonic polarization sensing of electrostatic superlattice potentials
• Photoluminescence Detection of Polytype Polarization in r-MoS2 Enabled by Asymmetric Dielectric Environments
• Enhancement of the WS${}_2$ A${}_{1\text{g}}$ Raman Mode in MoS${}_2$/WS${}_2$ Heterostructures
• Ferroelectric Control of Interlayer Excitons in 3R-MoS${}_2$ / MoSe${}_2$ Heterostructures
• Many-body description of two-dimensional van der Waals ferroelectric $\alpha -$In${}_2$Se${}_3$
• Investigating the Ferroelectric Potential Landscape of 3R-MoS${}_2$ through Optical Measurements
• Physical Pictures for Quasisymmetry in Crystals
• Superconducting cavity probes sliding ferroelectricity in small-angle twisted WSe${}_2$