Interlayer Interactions in Anisotropic Atomically-thin Rhenium Diselenide

Abstract

Recently, two-dimensional (2D) materials with strong in-plane anisotropic properties such as black phosphorus have demonstrated great potential for developing new devices that can take advantage of its reduced lattice symmetry with potential applications in electronics, optoelectronics and thermoelectrics. However, the selection of 2D material with strong in-plane anisotropy has so far been very limited and only sporadic studies have been devoted to transition metal dichalcogenides (TMDC) materials with reduced lattice symmetry, which is yet to convey the full picture of their optical and phonon properties, and the anisotropy in their interlayer interactions. Here, we study the anisotropic interlayer interactions in an important TMDC 2D material with reduced in-plane symmetry - atomically thin rhenium diselenide (ReSe2) - by investigating its ultralow frequency interlayer phonon vibration modes, the layer dependent optical bandgap, and the anisotropic photoluminescence (PL) spectra for the first time. The ultralow frequency interlayer Raman spectra combined with the first study of polarization-resolved high frequency Raman spectra in mono- and bi-layer ReSe2 allows deterministic identification of its layer number and crystal orientation. PL measurements show anisotropic optical emission intensity with bandgap increasing from 1.26 eV in the bulk to 1.32 eV in monolayer, consistent with the theoretical results based on first-principle calculations. The study of the layer-number dependence of the Raman modes and the PL spectra reveals the relatively weak van der Waals interaction and 2D quantum confinement in atomically-thin ReSe2.

17 pages, 5 figures, supplementary information

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• Polytypism and Unexpected Strong Interlayer Coupling of two-Dimensional Layered ReS2
• Strain-shear coupling in bilayer MoS2
• Monolayer Molybdenum Disulfide Nanoribbons with High Optical Anisotropy
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• Complete determination of crystallographic orientation of ReX2 (X=S, Se) by polarized Raman spectroscopy
• Direct versus indirect band gap emission and exciton-exciton annihilation in atomically thin molybdenum ditelluride (MoTe${}_2$)
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• Interlayer bond polarizability model for stacking-dependent low-frequency Raman scattering in layered materials
• Narrow-band anisotropic electronic structure of ReS${}_2$
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• Electronic bandstructure and van der Waals coupling of ReSe2 revealed by high-resolution angle-resolved photoemission spectroscopy
• Shear and breathing modes of layered materials
• Visualizing Orbital Content of Electronic Bands in Anisotropic 2D Semiconducting ReSe${}_2$
• Vibrational and dielectric properties of the bulk transition metal dichalcogenides
• The optical signature of few-layer ReSe${}_2$
• Electronic band structure of rhenium dichalcogenides
• Rigid-layer Raman-active modes in $N$-layer Transition Metal Dichalcogenides: interlayer force constants and hyperspectral Raman imaging
• Vibrational and dielectric properties of monolayer transition metal dichalcogenides
• Interplay of crystal thickness and in-plane anisotropy and evolution of quasi-one dimensional electronic character in ReSe${}_2$
• External screening and lifetime of exciton population in single-layer ReSe${}_2$ probed by time- and angle-resolved photoemission spectroscopy