Second Harmonic Generation in Atomically Thin MoTe₂

Abstract Optical second harmonic generations (SHGs) from atomically thin MoTe₂ flakes with 2H and 1T′ phases are studied. From 2H‐MoTe₂ samples with odd (even) numbers of layers, strong (negligible) SHGs are observed due to the layer‐dependent broken inversion symmetry. When pumped by a telecom‐band laser, SHG from a monolayer 2H‐MoTe₂ is about one order of magnitude stronger than that from a monolayer WS₂; an extremely high second‐order nonlinear susceptibility of 2.5 nm V⁻¹ is estimated, presenting the highest value among those reported in 2D materials. SHG measurements in MoTe₂ are also demonstrated as an efficient way to distinguish the 2H‐to‐1T′ phase transition. Compared with the SHG in 2H‐MoTe₂, 1T′‐MoTe₂'s SHG has much lower efficiency and the polarization dependence is changed from a six‐fold pattern to a two‐lobe pattern.