Nonlinear optical materials (NOMs) have attracted great attention among researchers in various areas such as optical frequency comb generation, [1,2] optical modulation, [3-5] and all-optical switching. [6,7] Since Franken et al. first observed the second harmonic generation in single crystalline quartz in 1961, [8] tremendous exciting results have been obtained based on various NOMs towards a variety of applications. In general, NOMs can be basically classified into second-order (LiNbO 3 , [9] LiTaO 3 , [10] KTP [11]), third-order (lnSb, [12] Si [13]), and