These high optical nonlinearities are emanating from the topological insulator character of the layers which can be observed in 2D structures. However, the relation between the structural characteristics of topological insulators and their optical nonlinearities is still not sufficiently explored. The target of the thesis is to shed light on the origins of the nonlinear optical properties of 2D topological insulators (like Sb2Te3, Bi2Te3 and Bi2Se3).