“…17 As evidenced in Figure 5, the non-zero SH value at β=0 and its dependence on β suggest the presence of some nanocrystals of 1 with orientation not perpendicular to the film surface. [20][21] We have evidence that the contribution of these not-oriented nanocrystals of 1 to the SH signal becomes more and more relevant with the number of cycles producing a decrease of the SHG signal, as expected for a decrease of the polar orientation of the nanocrystals of 1 by increasing the number of layers. The second order NLO coefficient d33 of the film after 4 and 9 cycles, obtained ex-situ by the standard Maker fringe method, is 0.57 and 2.10 pm/V, respectively.…”