“…The morphological, structural, optical, and chemical properties of the exfoliated BiTeI flakes are evaluated here through a combination of microscopic and spectroscopic techniques, including nonlinear optical microscopy for second-harmonic generation (SHG). In fact, the concurrent spin–orbit coupling and structural inversion asymmetry of Rashba-type materials manifest themselves in nonlinear optical signals whose characteristics can be defined or even correlated to the Rashba strength of the material. , Consequently, 2D Rashba-type materials potentially provide novel nanometer-thin platforms for nonlinear optical studies and applications. − In addition, as shown for other polar 2D materials, such as group-IV metal monochalcogenides, the lack of inversion symmetry and strong quantum confinement can lead to extraordinary second-order nonlinear optical effects . Even more, since the nanometric thickness of exfoliated materials is much smaller than the second-harmonic (SH) coherence length, 2D materials bypass phase-matching constraints encountered in 3D nonlinear crystals. , Thus, we measure SHG from few-layer BiTeI flakes, which exhibit a large nonlinear optical response 10-fold more intense than that of bulk BiTeI crystals and of the same order of magnitude as that of group VI monolayer transition metal dichalcogenides (TMDs) (|χ (2) | ∼0.1–1 nm V –1 ). , These results prove the potential of LPE-produced BiTeI as a solution-processable low-dimensional Rashba-type material.…”