Subscribe to the gold package and get unlimited access to Shamra Academy
Register a new userExamining Experimental Raman Mode Behavior in Mono- and Bi-layer 2H-TaSe$_{2}$ via Density Functional Theory
61
0
0.0
(
0
)
Ask ChatGPT about the research
No Arabic abstract
Tantalum diselenide (TaSe$_{2}$) is a metallic transition metal dichalcogenide whose equilibrium structure and vibrational behavior strongly depends on temperature and thickness, including the emergence of charge density wave (CDW) states at very low T. In this work, observed modes for mono- and bi-layer are described across several spectral regions and com-pared to the bulk ones. Such modes, including an experimentally observed forbidden Raman mode and low frequency CDW modes, are then matched to corresponding density functional theory (DFT) predicted vibrations, to unveil their inner working. The excellent match between experimental and computational results justifies the presented vibrational visualizations of these modes. Additional support is provided by experimental phonons seen in Raman spectra as a function of temperature and thickness. These results highlight the importance of understanding interlayer interactions and their effects on mode behaviors.
rate research
Read More
Metallic transition metal dichalcogenides like tantalum diselenide (TaSe$_{2}$) exhibit exciting behaviors at low temperatures, including the emergence of charge density wave (CDW) states. In this work, density functional theory (DFT) is used to investigate how structural, electronic, and Raman spectral properties of the CDW configuration change as a function of thickness. Such findings highlight the influence of dimensionality change (from 2D to 3D) and van der Waals (vdW) interactions on the system properties. The vdW effect is most strongly present in bulk TaSe$_{2}$ in the spectral range 165 cm$^{-1}$ to 215 cm$^{-1}$. The phonons seen in the experimental Raman spectra are compared with the results calculated from the DFT models as a function of temperature and layer number. The matching of data and calculations substantiates the models description of the CDW structural formation as a function of thickness, which is shown in depth for 1L through 6L systems. These results highlight the importance of understanding interlayer interactions, which are pervasive in many quantum phenomena involving two-dimensional confinement.
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.
We investigated interlayer phonon modes of mechanically exfoliated few-layer 2H-SnS2 samples by using room temperature low-frequency micro-Raman spectroscopy. Raman measurements were performed using laser wavelength of 441.6, 514.4, 532 and 632.8 nm with power below 100 uW and inside a vacuum chamber to avoid photo-oxidation. The intralayer Eg and A1g modes are observed at ~206 cm-1 and ~314 cm-1, respectively, but the Eg mode is much weaker for all excitation energies. The A1g mode exhibits strong resonant enhancement for the 532 nm (2.33 eV) laser. In the low-frequency region, interlayer vibrational modes of shear and breathing modes are observed. These modes show characteristic dependence on the number of layers. The strengths of the interlayer interactions are estimated by fitting the interlayer mode frequencies using the linear chain model and are found to be 1.64 x10^19 N.m-3 and 5.03 x10^19 N.m-3 for the shear and breathing modes, respectively.
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.
Charge-density-waves (CDW) which occur mainly in low-dimensional systems have a macroscopic wave function similar to superfluids and superconductors. Kosterlitz-Thouless (KT) transition is observed in superfluids and superconductors, but the presence of KT transition in ultra-thin CDW systems has been an open problem. We report the direct real-space observation of CDWs with new order states in mono-, bi-, and tri-layer 1T-TaS_2 crystal by using a low voltage scanning-transmission-electron-microscope (STEM) without a substrate. This method is ideal to observe local atomic structures and possible defects. We clearly observed that the mono-layer crystal has a new triclinic stripe CDW order without the triple q condition q_1 + q_2 + q_3 = 0. A strong electron-phonon interaction gives rise to new crevasse (line) type defects instead of disclination (point) type defects due to the KT transition. These results reaffirm the importance of the electron-phonon interaction in mono-layer nanophysics.
Log in to be able to interact and post comments
comments
Fetching comments
Sign in to be able to follow your search criteria
