Excitonic signatures of ferroelectric order in parallel-stacked MoS2

Swarup Deb (), Johannes Krause, Paulo E. Faria Junior, Michael Andreas Kempf, Rico Schwartz, Kenji Watanabe, Takashi Taniguchi, Jaroslav Fabian and Tobias Korn ()
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Swarup Deb: University of Rostock
Johannes Krause: University of Rostock
Paulo E. Faria Junior: University of Regensburg
Michael Andreas Kempf: University of Rostock
Rico Schwartz: University of Rostock
Kenji Watanabe: NIMS
Takashi Taniguchi: NIMS
Jaroslav Fabian: University of Regensburg
Tobias Korn: University of Rostock

Nature Communications, 2024, vol. 15, issue 1, 1-8

Abstract: 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-MoS2 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 direct correspondence between spin-valley dynamics and stacking order.

Date: 2024
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DOI: 10.1038/s41467-024-52011-3

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