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Free carrier absorption (FCA) is established to be the cause of nonlinear losses in plasma‐enhanced chemical vapor deposition (PECVD) silicon‐rich nitride (SRN) waveguides. To validate this hypothesis, a photo‐induced current is measured in SRN thin films with refractive indices varying between 2.5 and 3.15 when a C‐band laser light is illuminating the SRN films at various powers, indicating the generation of free carriers. Furthermore, nonlinear loss dynamics is, for the first time, measured and characterized in detail in SRN waveguides by utilizing high peak power C‐band complex shape optical pulses for estimation of free carrier generation (FCG) and free carrier recombination (FCR) lifetimes and their dynamics. Both FCG and FCR are found to decrease with an increase in the refractive index of SRN, and, specifically, the FCR lifetimes are found (92 ± 7) ns, (39 ± 3) ns, and (31 ± 2) ns for the SRN indices of 2.7, 3, and 3.15, respectively. Lastly, nonlinear losses in high refractive index SRN waveguides are demonstrated to be minimized and altogether avoided when the pulse duration reduced below the free carrier generation lifetime, thus providing a way of taking a full advantage of the large inherent SRN nonlinear properties. 

Silicon nitride is widely used in integrated photonics for optical nonlinear wave mixing due to its low optical losses combined with relatively high nonlinear optical properties and a wide‐range transparency window. It is known that a higher concentration of Si in silicon‐rich nitride (SRN) magnifies both the nonlinear response and optical losses, including nonlinear losses. To address the trade‐off, four‐wave mixing (FWM) is implemented in over a hundred SRN waveguides prepared by plasma‐enhanced chemical vapor deposition in a wide range of SRN refractive indices varying between 2.5 and 3.2 (measured in the C‐band). It is determined that SRN with a refractive index of about 3 maximizes the FWM efficiency for continuous‐wave operation, indicating that the refractive index of SRN is indeed a crucial optimization parameter for nonlinear optics applications. The FWM efficiency is limited by large nonlinear optical losses observed in SRN waveguides with indices larger than 2.7, which are not related to two‐photon absorption. Finally, the third‐order susceptibility and the nonlinear refractive index are estimated for multiple SRN refractive indices, and, specifically, the nonlinearities as large as and are estimated in a waveguide with an SRN refractive index of 3.2.