Jiang-Bin Wu

Raman spectroscopy of shear and layer breathing modes in multilayer MoS2

We study by Raman scattering the shear and layer breathing modes in multilayer MoS2. These are identified by polarization measurements and symmetry analysis. Their positions change significantly with the number of layers, with different scaling for odd and even layers. A chain model can explain the results, with general applicability to any layered material, allowing a reliable diagnostic of their thickness.

Resonant Raman spectroscopy of twisted multilayer graphene

Graphene and other two-dimensional crystals can be combined to form various hybrids and heterostructures, creating materials on demand, in which the interlayer coupling at the interface leads to modified physical properties as compared to their constituents. Here, by measuring Raman spectra of shear modes, we probe the coupling at the interface between two artificially-stacked few-layer graphenes rotated with respect to each other. The strength of interlayer coupling between the two interface layers is found to be only 20% of that between Bernal-stacked layers. Nevertheless, this weak coupling manifests itself in a Davydov splitting of the shear mode frequencies in systems consisting of two equivalent graphene multilayers, and in the intensity enhancement of shear modes due to the optical resonance with several optically allowed electronic transitions between conduction and valence bands in the band structures. This study paves way for fundamental understanding into the interface coupling of two-dimensional hybrids and heterostructures.Graphene and other two-dimensional crystals can be combined to form various hybrids and heterostructures, creating materials on demand with properties determined by the interlayer interaction. This is the case even for a single material, where multilayer stacks with different relative orientation have different optical and electronic properties. Probing and understanding the interface coupling is thus of primary importance for fundamental science and applications. Here we study twisted multilayer graphene flakes with multi-wavelength Raman spectroscopy. We find a significant intensity enhancement of the interlayer coupling modes (C peaks) due to resonance with new optically allowed electronic transitions, determined by the relative orientation of the layers. The interlayer coupling results in a Davydov splitting of the C peak in systems consisting of two equivalent graphene multilayers. This allows us to directly quantify the interlayer interaction, which is much smaller compared with Bernal-stacked interfaces. This paves the way to the use of Raman spectroscopy to uncover the interface coupling of two-dimensional hybrids and heterostructures.

Interlayer Interactions in Anisotropic Atomically-thin Rhenium Diselenide

In this work, we study the interlayer phonon vibration modes, the layer-numberdependent optical bandgap, and the anisotropic photoluminescence (PL) spectra of atomically thin rhenium diselenide (ReSe2) for the first time. The ultralow frequency interlayer Raman spectra and the polarization-resolved high frequency Raman spectra in ReSe2 allow the identification of its layer number and crystal orientation. Furthermore, PL measurements show the anisotropic optical emission intensity of the material with its bandgap increasing from 1.26 eV in the bulk to 1.32 eV in the monolayer. The study of the layer-number dependence of the Raman modes and the PL spectra reveals relatively weak van der Waal’s interaction and two-dimensional (2D) quantum confinement in the atomically thin ReSe2. The experimental observation of the intriguing anisotropic interlayer interaction and tunable optical transition in monolayer and multilayer ReSe2 establishes the foundation for further exploration of this material in the development of anisotropic optoelectronic devices functioning in the near-infrared spectrum, which is important for many applications in optical communication and infrared sensing.

Interface Coupling in Twisted Multilayer Graphene by Resonant Raman Spectroscopy of Layer Breathing Modes

Raman spectroscopy is the prime nondestructive characterization tool for graphene and related layered materials. The shear (C) and layer breathing modes (LBMs) are due to relative motions of the planes, either perpendicular or parallel to their normal. This allows one to directly probe the interlayer interactions in multilayer samples. Graphene and other two-dimensional (2d) crystals can be combined to form various hybrids and heterostructures, creating materials on demand with properties determined by the interlayer interaction. This is the case even for a single material, where multilayer stacks with different relative orientations have different optical and electronic properties. In twisted multilayer graphene there is a significant enhancement of the C modes due to resonance with new optically allowed electronic transitions, determined by the relative orientation of the layers. Here we show that this applies also to the LBMs, which can be now directly measured at room temperature. We find that twisting has a small effect on LBMs, quite different from the case of the C modes. This implies that the periodicity mismatch between two twisted layers mostly affects shear interactions. Our work shows that ultralow-frequency Raman spectroscopy is an ideal tool to uncover the interface coupling of 2d hybrids and heterostructures.

Substrate-free layer-number identification of two-dimensional materials: A case of Mo0.5W0.5S2 alloy

Any of two or more two-dimensional (2D) materials with similar properties can be alloyed into a new layered material, namely, 2D alloy. Individual monolayer in 2D alloys is kept together by van der Waals interactions. The property of multilayer alloys is a function of their layer number. Here, we studied the shear (C) and layer-breathing (LB) modes of Mo0.5W0.5S2 alloy flakes and their link to the layer number. The study reveals that the disorder effect is absent in the C and LB modes of 2D alloys, and the monatomic chain model can be used to estimate the frequencies of the C and LB modes. We demonstrated how to use the frequencies of C and LB modes to identify the layer number of alloy flakes deposited on different substrates. This technique is independent of the substrate, stoichiometry, monolayer thickness, and complex refractive index of 2D materials, offering a robust and substrate-free approach for layer-number identification of ultrathin flakes of 2D materials, such as 2D crystals and 2D alloys.

Ultralow-frequency shear modes of 2-4 layer graphene observed in scroll structures at edges

The in-plane shear modes between neighbor-layers of 2-4 layer graphenes (LGs) and the corresponding graphene scrolls rolled up by 2-4LGs were investigated by Raman scattering. In contrast to that just one shear mode was observed in 3-4LGs, all the shear modes of 3-4LGs were observed in 3-4 layer scrolls (LSs), whose frequencies agree well with the theoretical predication by both a force-constant model and a linear chain model. In comparison to the broad width (about 12cm

Interfacial Interactions in van der Waals Heterostructures of MoS2 and Graphene

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Monolayer Molybdenum Disulfide Nanoribbons with High Optical Anisotropy

) for the G band in graphite, all the shear modes exhibit an intrinsic line width of about 1.0 cm

Ultralow-frequency Raman system down to 10 cm−1 with longpass edge filters and its application to the interface coupling in t(2+2)LGs

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The Pentagonal Nature of Self-Assembled Silicon Chains and Magic Clusters on Ag(110)

. The local electronic structures dependent on the local staking configurations enhance the intensity of the shear modes in corresponding 2-4LSs zones, which makes it possible to observe all the shear modes. It provides a direct evidence that how the band structures of FLGs can be sensitive to local staking configurations. This result can be extended to n layer graphene (n > 4) for the understanding of the basic phonon properties of multi-layer graphenes. This observation of all-scale shear modes can be foreseen in other 2D materials with similar scroll structures.