Discovering the forbidden Raman modes at the edges of layered materials

The edges of layered materials have unique properties that substantially differ from the body regions. In this work, we perform a systematic Raman study of the edges of various layered materials (MoS2, WS2, WSe2, PtS2, and black phosphorus). The Raman spectra of the edges feature newly observed forbidden Raman modes, which are originally undetectable from the body region. By selecting the edge type and the polarization directions of the incident and scattered light, all forbidden Ramanmodes are distinctly detected. Optical simulations show that the edges of layered materials drastically distort the electromagnetic fields of both the incident and scattered light, so that the light interacts with the edges in a distinct way, which differs from its interactions with the body regions.