Raman‐Active Interlayer Phonons and Moiré Phonons in Twisted Thin‐Layer MoTe2

Abstract

AbstractA wide range of artificially twist‐stacked van der Waals materials offer versatile building blocks for quantum optoelectronic devices. Among these, twisted bilayer MoTe2 has excellent optical properties in the near‐infrared range and can be integrated with silicon photonics. While recent studies mainly focus on the emission properties in twisted bilayer MoTe2, a comprehensive investigation of how Moiré superlattice affects phonon modes in twisted thin‐layer MoTe2 remains unexplored. These phonon modes can serve as indicators of stacking configuration and interface uniformity. Here, a series of twisted bilayer and tetralayer MoTe2 with precisely controlled twist angles ranging from 0° to 60° are prepared. Using polarization‐dependent low‐frequency Raman spectroscopy, the evolution of interlayer phonon modes at different twist angles is identified. Additionally, a range of acoustic phonon modes activated by Moiré potentials in both twisted bilayer MoTe2 and twisted tetralayer MoTe2 are observed and analyzed. The findings provide experimental evidence of the interlayer phonon coupling and Moiré phonons in MoTe2, offering insights for the future development of near‐infrared optoelectronic devices based on twisted thin‐layer MoTe2.