| Changgu Lee1, Hugen Yan2, Louis E. Brus3, Tony F. Heinz2,4, James Hone1, Sunmin Ryu5*
This study investigates the lattice vibrations of single and few-layer MoS₂ using Raman spectroscopy and atomic-force microscopy (AFM). MoS₂ samples were exfoliated onto SiO₂/Si substrates and characterized by Raman spectroscopy. The number of layers was determined by AFM, revealing a thickness-dependent shift in Raman modes. The E₁₂g mode frequency decreases with increasing thickness, while the A₁g mode frequency increases. These shifts are not solely due to van der Waals interactions but are also influenced by Coulombic interactions and changes in intralayer bonding. The frequency difference between the two modes serves as a reliable indicator of layer thickness. The results demonstrate that the structural parameters of layered materials evolve as they transition from 3D to 2D. MoS₂, a stable layered metal dichalcogenide, has potential applications in catalysis, lubrication, and photovoltaics. The study highlights the sensitivity of Raman spectroscopy to layer thickness and provides insights into the effects of interlayer interactions on vibrational properties. The findings suggest that stacking-induced changes in intralayer bonding and Coulombic interactions play a significant role in the vibrational behavior of MoS₂. The research also shows that Raman intensity and linewidth vary with layer thickness, indicating the influence of electronic structure and surface effects. The study underscores the importance of understanding interlayer interactions in 2D materials and provides a method for determining layer thickness with atomic precision.This study investigates the lattice vibrations of single and few-layer MoS₂ using Raman spectroscopy and atomic-force microscopy (AFM). MoS₂ samples were exfoliated onto SiO₂/Si substrates and characterized by Raman spectroscopy. The number of layers was determined by AFM, revealing a thickness-dependent shift in Raman modes. The E₁₂g mode frequency decreases with increasing thickness, while the A₁g mode frequency increases. These shifts are not solely due to van der Waals interactions but are also influenced by Coulombic interactions and changes in intralayer bonding. The frequency difference between the two modes serves as a reliable indicator of layer thickness. The results demonstrate that the structural parameters of layered materials evolve as they transition from 3D to 2D. MoS₂, a stable layered metal dichalcogenide, has potential applications in catalysis, lubrication, and photovoltaics. The study highlights the sensitivity of Raman spectroscopy to layer thickness and provides insights into the effects of interlayer interactions on vibrational properties. The findings suggest that stacking-induced changes in intralayer bonding and Coulombic interactions play a significant role in the vibrational behavior of MoS₂. The research also shows that Raman intensity and linewidth vary with layer thickness, indicating the influence of electronic structure and surface effects. The study underscores the importance of understanding interlayer interactions in 2D materials and provides a method for determining layer thickness with atomic precision.