Unveiling the origin of anomalous low-frequency Raman mode in CVD-grown monolayer WS 2

Substrates provide the necessary support for scientific explorations of numerous promising features and exciting potential applications in two-dimensional (2D) transition metal dichalcogenides (TMDs). To utilize substrate engineering to alter the properties of 2D TMDs and avoid introducing unwanted adverse effects, various experimental techniques, such as high-frequency Raman spectroscopy, have been used to understand the interactions between 2D TMDs and substrates. However, sample-substrate interaction in 2D TMDs is not yet fully understood due to the lack of systematic studies by techniques that are sensitive to 2D TMD-substrate interaction. This work systematically investigates the interaction between tungsten disulfide (WS 2 ) monolayers and substrates by low-frequency Raman spectroscopy, which is very sensitive to WS 2 -substrate interaction. Strong coupling with substrates is clearly revealed in chemical vapor deposition (CVD)-grown monolayer WS 2 by its low-wavenumber interface mode. It is demonstrated that the enhanced sample-substrate interaction leads to tensile strain on monolayer WS 2 , which is induced during the cooling process of CVD growth and could be released for monolayer WS 2 sample after transfer or fabricated by an annealing-free method such as mechanical exfoliation. These results not only suggest the effectiveness of low-frequency Raman spectroscopy for probing sample-substrate interactions in 2D TMDs, but also provide guidance for the design of high-performance devices with the desired sample-substrate coupling strength based on 2D TMDs.