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Register a new userDouble resonance Raman modes in mono- and few-layer MoTe$_2$
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We study the second-order Raman process of mono- and few-layer MoTe$_2$, by combining {em ab initio} density functional perturbation calculations with experimental Raman spectroscopy using 532, 633 and 785 nm excitation lasers. The calculated electronic band structure and the density of states show that the electron-photon resonance process occurs at the high-symmetry M point in the Brillouin zone, where a strong optical absorption occurs by a logarithmic Van-Hove singularity. Double resonance Raman scattering with inter-valley electron-phonon coupling connects two of the three inequivalent M points in the Brillouin zone, giving rise to second-order Raman peaks due to the M point phonons. The predicted frequencies of the second-order Raman peaks agree with the observed peak positions that cannot be assigned in terms of a first-order process. Our study attempts to supply a basic understanding of the second-order Raman process occurring in transition metal di-chalcogenides (TMDs) and may provide additional information both on the lattice dynamics and optical processes especially for TMDs with small energy band gaps such as MoTe$_2$ or at high laser excitation energy.
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We report two new first-order Raman modes in the spectra of few-layer MoS$_2$ at 286~cm$^{-1}$ and 471~cm$^{-1}$ for excitation energies above 2.4~eV. These modes appear only in few-layer MoS$_2$; therefore their absence provides an easy and accurate method to identify single-layer MoS$_2$. We show that these modes are related to phonons that are not observed in the single layer due to their symmetry. Each of these phonons leads to several nearly degenerate phonons in few-layer samples. The nearly degenerate phonons in few-layer materials belong to two different symmetry representations, showing opposite behavior under inversion or horizontal reflection. As a result, Raman active phonons exist in few-layer materials that have nearly the same frequency as the symmetry forbidden phonon of the single layer. We provide here a general treatment of this effect for all few-layer two-dimensional crystal structures with an inversion center or a mirror plane parallel to the layers. We show that always nearly degenerate phonon modes of different symmetry must occur and, as a result, similar pseudo-activation effects can be excepted.
The optical properties of the two-dimensional (2D) crystals are dominated by tightly bound electron-hole pairs (excitons) and lattice vibration modes (phonons). The exciton-phonon interaction is fundamentally important to understand the optical properties of 2D materials and thus help develop emerging 2D crystal based optoelectronic devices. Here, we presented the excitonic resonant Raman scattering (RRS) spectra of few-layer WS$_2$ excited by 11 lasers lines covered all of A, B and C exciton transition energies at different sample temperatures from 4 to 300 K. As a result, we are not only able to probe the forbidden phonon modes unobserved in ordinary Raman scattering, but also can determine the bright and dark state fine structures of 1s A exciton. In particular, we also observed the quantum interference between low-energy discrete phonon and exciton continuum under resonant excitation. Our works pave a way to understand the exciton-phonon coupling and many-body effects in 2D materials.
Two-dimensional crystals of semimetallic van der Waals materials hold much potential for the realization of novel phases, as exemplified by the recent discoveries of a polar metal in few layer 1T-WTe$_2$ and of a quantum spin Hall state in monolayers of the same material. Understanding these phases is particularly challenging because little is known from experiment about the momentum space electronic structure of ultrathin crystals. Here, we report direct electronic structure measurements of exfoliated mono-, bi-, and few-layer 1T-WTe$_2$ by laser-based micro-focus angle resolved photoemission. This is achieved by encapsulating with monolayer graphene a flake of WTe$_2$ comprising regions of different thickness. Our data support the recent identification of a quantum spin Hall state in monolayer 1T-WTe$_2$ and reveal strong signatures of the broken inversion symmetry in the bilayer. We finally discuss the sensitivity of encapsulated samples to contaminants following exposure to ambient atmosphere.
The Raman selection rules arise from the crystal symmetry and then determine the Raman activity and polarization of scattered phonon modes. However, these selection rules can be broken in resonant process due to the strong electron-phonon coupling effect. Here we reported the observation of breakdown of Raman selection rules in few-layer WS$_2$ by using resonant Raman scattering with dark A exciton. In this case, not only the infrared active modes and backscattering forbidden modes are observed, but the intensities of all observed phonon modes become strongest under paralleled-polarization and independent on the Raman tensors of phonons. We attributed this phenomenon to the interaction between dark A exciton and the scatted phonon, the so-called intraband Fr{o}hlich interaction, where the Raman scattering possibility is totally determined by the symmetry of exciton rather than the phonons due to strong electron-phonon coupling. Our results not only can be used to easily detect the optical forbidden excitonic and phononic states but also provide a possible way to manipulate optical transitions between electronic levels.
ReS$_2$ has recently emerged as a new member in the rapidly growing family of two-dimensional materials. Unlike MoS$_2$ or WSe$_2$, the optical and electrical properties of ReS$_2$ are not isotropic due to the reduced symmetry of the crystal. Here, we present layer-dependent Raman measurements of ReS$_2$ samples ranging from monolayers to ten layers in the ultralow frequency regime. We observe layer breathing and shear modes which allow for easy assignment of the number of layers. Polarization-dependent measurements give further insight into the crystal structure and reveal an energetic shift of the shear mode which stems from the in-plane anisotropy of the shear modulus in this material.
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