Polytypism and Unexpected Strong Interlayer Coupling of two-Dimensional Layered ReS2

Abstract

The anisotropic two-dimensional (2D) van der Waals (vdW) layered materials, with both scientific interest and potential application, have one more dimension to tune the properties than the isotropic 2D materials. The interlayer vdW coupling determines the properties of 2D multi-layer materials by varying stacking orders. As an important representative anisotropic 2D materials, multilayer rhenium disulfide (ReS2) was expected to be random stacking and lack of interlayer coupling. Here, we demonstrate two stable stacking orders (aa and a-b) of N layer (NL, N>1) ReS2 from ultralow-frequency and high-frequency Raman spectroscopy, photoluminescence spectroscopy and first-principles density functional theory calculation. Two interlayer shear modes are observed in aa-stacked NL-ReS2 while only one interlayer shear mode appears in a-b-stacked NL-ReS2, suggesting anisotropic-like and isotropic-like stacking orders in aa- and a-b-stacked NL-ReS2, respectively. The frequency of the interlayer shear and breathing modes reveals unexpected strong interlayer coupling in aa- and a-b-NL-ReS2, the force constants of which are 55-90% to those of multilayer MoS2. The observation of strong interlayer coupling and polytypism in multi-layer ReS2 stimulate future studies on the structure, electronic and optical properties of other 2D anisotropic materials.

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• Stacking-Dependent Interlayer Phonons in 3R and 2H MoS${}_2$
• Interlayer bond polarizability model for stacking-dependent low-frequency Raman scattering in layered materials
• Polytypism in Few-Layer Gallium Selenide
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• Interlayer Coupling in Two-Dimensional Semiconductor Materials
• Charge tunable structural phase transitions in few-layer tellurium: a step toward building mono-elemental devices
• Non equilibrium anisotropic excitons in atomically thin ReS${}_2$
• Phase Modulators Based on High Mobility Ambipolar ReSe2 Field-Effect Transistors
• Breakdown of Raman Selection Rules By Fröhlich Interaction in Few-Layer WS${}_2$
• Rigid-layer Raman-active modes in $N$-layer Transition Metal Dichalcogenides: interlayer force constants and hyperspectral Raman imaging
• Two-dimensional ReS2: Solution to the Unresolved Queries on Its Structure and Inter-layer Coupling Leading to Potential Optical Applications
• Reliable and Broad-range Layer Identification of Au-assisted Exfoliated Large Area MoS${}_2$ and WS${}_2$ Using Reflection Spectroscopic Fingerprints
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• Doping controlled Fano resonance in bilayer 1T${}^{\prime }$-ReS${}_2$: Raman experiments and first-principles theoretical analysis
• Linear Dichroism Conversion in Quasi One-Dimensional Perovskite Chalcogenide
• Two ultra-stable novel allotropes of Tellurium few-layers
• Unraveling the Photophysics of Liquid-Phase Exfoliated Two-Dimensional ReS2 Nanoflakes