Physical origin of Davydov splitting and resonant Raman spectroscopy of Davydov components in multilayer MoTe2

Abstract

We systematically study the high-resolution and polarized Raman spectra of multilayer (ML) MoTe2. The layer-breathing (LB) and shear (C) modes are observed in the ultralow-frequency region, which are used to quantitatively evaluate the interlayer coupling in ML MoTe2 based on the linear chain model, in which only the nearest interlayer coupling is considered. The Raman spectra on three different substrates verify the negligible substrate effect on the phonon frequencies of ML MoTe2. Ten excitation energies are used to measure the high-frequency modes of N-layer MoTe2 (NL MoTe2; N is an integer). Under the resonant excitation condition, we observe N-dependent Davydov components in ML MoTe2 , originating from the Raman-active A'1(A21g) modes at ~172 cm-1. More than two Davydov components are observed in NL MoTe2 for N larger than 4 by Raman spectroscopy. The N-dependent Davydov components are further investigated based on the symmetry analysis. A van der Waals model only considering the nearest interlayer coupling has been proposed to well understand the Davydov splitting of high-frequency A'1(A21g) modes. The different resonant profiles for the two Davydov components in 3L MoTe2 indicate that proper excitation energy of ~1.8-2.2 eV must be chosen to observe the Davydov splitting in ML MoTe2 . Our work presents a simple way to identify layer number of ultrathin MoTe2 flakes by the corresponding number and peak position of Davydov components. Our work also provides a direct evidence from Raman spectroscopy of how the nearest van der Waals interactions significantly affect the frequency of the high-frequency intralayer phonon modes in multilayer MoTe2 and expands the understanding on the lattice vibrations and interlayer coupling of transition metal dichalcogenides and other two-dimensional materials.