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Interfacial ferroelectricity is a phenomenon arising in a plethora of parallel-stacked layered materials,in which out-of-plane ferroelectric order is switched by in-plane sliding of adjacent layers. Unlike conventional ferroelectrics, interfacial ferroelectricity is stable against doping, potentially enabling next-generation devices with storage and computational capabilities.12 However, the field has been limited to indirect sensingor visualizing the ferroelectricity in basic bilayer units employing surface-sensitive probes. In the case of transition metal dichalcogenides, this leaves a void of in-depth knowledge about the influence of ferroelectric order on their intrinsic valley and excitonic properties. Here, we report direct far-field probing of ferroelectricity in few-layer 3R-MoS2 using reflectance contrast spectroscopy. Contrary to a simple electrostatic perception, the intralayer excitons with strictly in-plane dipole orientation are sensitive to out-of-plane ferroelectric ordering. On the other hand, despite possessing an out-of-plane electric dipole component, layer-hybridized momentum-indirect excitons remain decoupled from such ordering. Ab initio calculations elucidate the microscopic origin of the correspondence between ferroelectric order and optical response. Using a field-effect device, we demonstrate room temperature control and optical readout of multi-state polarization and its hysteretic switching. Time-resolved Kerr ellipticity measured in different ferroelectric domains reveals a direct correspondence between spin-valley dynamics and ferroelectric order.
Subject Terms Physical sciences/Nanoscience and technology/Nanoscale materials/Two-dimensional materials

Rights:

• Creative Commons BY Attribution 4.0 International
  

Keyword: Interfacial ferroelectricity, valley properties, reflectance contrast

Date published: 2024-08-31

Publisher: Springer Science and Business Media LLC

Journal:

• Nature Communications (ISSN: 20411723) vol. 15 issue. 1 7595

Funding:

• JSPS KAKENHI
• Deutsche Forschungsgemeinschaft 314695032
• Deutsche Forschungsgemeinschaft 441234705
• Deutsche Forschungsgemeinschaft 443361515
• Deutsche Forschungsgemeinschaft 467549803
• Alexander von Humboldt-Stiftung
• Deutsche Forschungsgemeinschaft 441219355

Manuscript type: Publisher's version (Version of record)

MDR DOI:

First published URL: https://doi.org/10.1038/s41467-024-52011-3

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Updated at: 2025-02-27 16:30:36 +0900

Published on MDR: 2025-02-27 16:30:36 +0900