Note that the previous observations of the E and A1 modes were based on a sample prepared under ambient conditions, quickly after the deposition of the Au layers, where the processing time caused partial saturation of the Au layer surface. As a result, the magnitude of the MoS2-metal interaction was reduced from the unperturbed value, and subsequently, the corresponding Raman modes decreased in intensity. Consequently, in our previous study , the latter Raman modes were observed only by exploiting the strong nearfield enhancement of tipenhanced Raman measurements. Here, the UHV conditions preserved the reactivity of the fresh metal surface and caused strong binding of the MoS2 layer to the metal, resulting in an exfoliation process with a yield of nearly 100% (Figures and). The uniformity of the interaction over the layer was confirmed by the statistical analysis of the obtained Raman spectra from 50×50 µm 2 maps performed at different positions of the samples as shown in the Supplementary Figure .