N-layer transition metal dichalcogenides provide a unique platform to investigate the evolution of the physical properties between the bulk (three dimensional) and monolayer (quasi two-dimensional) limits. Here, using high-resolution micro-Raman spectroscopy, we report a unified experimental description of the Γ-point optical phonons in N-layer 2H-molybdenum ditelluride (MoTe2). We observe a series of N-dependent low-frequency interlayer shear and breathing modes (below 40cm−1, denoted LSM and LBM) and well-defined Davydov splittings of the mid-frequency modes (in the range 100−200cm−1, denoted iX and oX), which solely involve displacements of the chalcogen atoms. In contrast, the high-frequency modes (in the range 200−300cm−1, denoted iMX and oMX), arising from displacements of both the metal and chalcogen atoms, exhibit considerably reduced splittings. The manifold of phonon modes associated with the in-plane and out-of-plane displacements are quantitatively described by a force constant model, including interactions up to the second nearest neighbor and surface effects as fitting parameters. The splittings for the iX and oX modes observed in N-layer crystals are directly correlated to the corresponding bulk Davydov splittings between the E2u/E1g and B1u/A1g modes, respectively, and provide a measurement of the frequencies of the bulk silent E2u and B1u optical phonon modes. Our analysis could readily be generalized to other layered crystals.
@article{arxiv.1509.02823,
title = {Unified description of the optical phonon modes in $N$-layer MoTe$_2$},
author = {Guillaume Froehlicher and Etienne Lorchat and François Fernique and Chaitanya Joshi and Alejandro Molina-Sánchez and Ludger Wirtz and Stéphane Berciaud},
journal= {arXiv preprint arXiv:1509.02823},
year = {2016}
}
Comments
Main Text (5 Figures, 2 Tables) + Supporting Information (12 Figures)