Nonstoichiometric SiN x with enhancing optical nonlinearity is enabled to facilitate the waveguide microring resonator for cross-wavelength all-optical data processing applications. The Si/N composition ratio of the nonstoichiometric SiN x can be detuned from stoichiometric to Si-rich by adjusting the SiH 4 /NH 3 fluence ratios. Under pumping with incoming pulsed data, the comb-like transmittance of the nonstoichiometric SiN x microring resonator can spectrally red-shift by 100 pm as its effective refractive index changed by more than 1 order of magnitude due to the enhanced nonlinear Kerr effect. The enlarged refractive index of Δn = 1.6 × 10 −4 with increasing nonlinear refractive index to n 2 = 1.6 × 10 −13 cm 2 /W at 1550 nm is observed at a Si concentration of 66.2% in the Si-rich SiN x film. In application, a cross-wavelength all-optical data conversion/inversion processor based on the nonstoichiometric SiN x microring resonator is presented. The dense nanoscale Si content formed by a higher Si/N composition ratio of the SiN x contributes to an enhanced Kerr effect based optical nonlinear switching, which enables the optimized 12 Gbit/s all-optical conversion of the pulsed return-to-zero on−off-keying (RZ-OOK) data with converted or inverted format. The photon lifetime of ∼19 ps in the Si-rich SiN x microring resonator cavity can support the Si-rich SiN x alloptical Kerr switch with a maximal bandwidth of up to 50 GHz. S ilicon photonics has been considered to realize the optical interconnect circuits for decades, and the pure Si-based waveguide devices have played important roles in acting as different functionalities in this field. With the free-carrierinduced plasma dispersion effect, 1,2 a pure Si-based electrooptical modulator and all-optical modulators were demonstrated. 3−7 The all-optical modulation bandwidth extended from hundreds of MHz to several GHz but was limited by the carrier diffusion dominated lifetime of the bulk Si. 8,9 Recently, the free-carrier absorption (FCA) cross-section in the silicon quantum dots (Si-QDs) has been proved to be 1 order of magnitude larger than that in the bulk Si. 10−12 Even though shrinking the Si-QD size can further shorten the carrier relaxation lifetime due to the quantum confinement effect, 13,14 the effective free-carrier lifetime in Si-QDs is still much longer than that of the bulk Si so as to limit the modulation bandwidth of the Si-QD-based FCA modulator at around 1 MHz. 15−17 To develop an ultrafast all-optical modulator that is fully compatible with Si-based CMOS integrated circuits, the most appropriate solution among versatile approaches is to use the enhanced optical nonlinearity of the Si-QDs. Recently, the optical nonlinearity of the Si-QDs doped in SiO x has been analyzed by using the femtosecond Z-scan method. 18−21 The nonlinear Kerr coefficient of the Si-QDs is experimentally proved to be 2 orders of magnitude higher than that of the bulk Si due to the strong quantum confinement effect. 18−22 The excitons generated in the highly confined Si-QDs...