Low-frequency Raman signature of Ag-intercalated few-layer MoS$_2$

TL;DR

This study combines theoretical calculations and experiments to show how silver intercalation in few-layer MoS$_2$ alters low-frequency Raman modes, enabling silver concentration assessment and interface quality characterization.

Contribution

It introduces a semi-classical model for multilayer MoS$_2$ with silver intercalation and demonstrates how low-frequency Raman spectroscopy can quantify silver content and interface quality.

Findings

Silver causes red-shifts in low-frequency Raman modes.

Raman spectroscopy can determine silver concentration.

The semi-classical model predicts vibrational behavior in multilayer systems.

Abstract

Density functional theory based calculations and experimental analysis on a limited number of real samples are performed to study how the presence of silver intercalated in the van der Waals gap of few-layer MoS$_2$ affects the low-frequency Raman active modes of this material. Silver is found to predominantly affect the breathing-like and shear-like vibrational modes of MoS$_2$. These modes correspond to quasi-rigid movements of each individual layer with a restoring force (and, in turn, frequency) that is determined by modulations in the weak interlayer interactions. Noticeable red-shifts with increasing Ag concentration are found for all low-frequency modes. This finding indicates the potential for low-frequency vibrations as useful gauges for practical determination of silver concentration using low-frequency Raman spectroscopy. This work also describes a semi-classical linear chain model that allows to extrapolate results to a large number of layers. Further, first-principles calculations show how Raman spectroscopy can be used to characterize the quality of the two-dimensional interface between MoS$_2$ and a silver substrate.