Silicon nitride has emerged as a prominent platform for building photonics integrated circuits. While its nonlinear properties based on third-order effects have been successfully exploited, an efficient second harmonic generation in standard stoichiometric silicon nitride (Si3N4) waveguides can also be achieved after all-optical poling, as was recently shown. The root of such a phenomenon has been attributed to the inscription of a self-organized periodic space-charge grating along the waveguide, allowing an effective χ(2) and automatic quasi-phase-matching of pump and second harmonic. However, the different parameters and their role in increasing the efficiency of the process are still not fully comprehended. In this work, we use optical means to identify the general conditions of mode matching occurring during all-optical poling. The overlap integral between pump and second harmonic optical modes is shown to be the governing parameter in determining the features of the χ(2) gratings. Two-photon microscopy measurements of the χ(2) gratings reveal the presence of a secondary periodicity in some of the waveguides used in the study. According to overlap integral simulations, such an effect can occur due to mode mixing in the waveguide bends. From a study of poling dynamics, we observe that poling efficiency and rate increase as a function of optical pump power and waveguide length. However, in order to initiate poling, a critical pump intensity, which is lower for longer waveguides, must be coupled into a waveguide. Temporal and thermal stability tests reveal the nature of charge traps responsible for grating inscription. After applying thermally activated hopping as a conductivity mechanism in our samples, we show that only shallow traps seem to be activated during the all-optical poling process.

Quasi-phase-matching has long been a widely used approach in nonlinear photonics, enabling efficient parametric frequency conversions such as second-harmonic generation. However, in silicon photonics the task remains challenging, as materials best suited for photonic integration lack second-order susceptibility (χ(2)), and means for achieving momentum conservation are limited. Here we present optically reconfigurable quasi-phase-matching in large-radius silicon nitride microresonators, resulting in up to 12.5-mW on-chip second-harmonic generated power and a conversion efficiency of 47.6% W−1. Most importantly, we show that such all-optical poling can occur unconstrained from intermodal phase-matching, leading to broadly tunable second-harmonic generation. We confirm the phenomenon by two-photon imaging of the inscribed χ(2) grating structures within the microresonators as well as by in situ tracking of both the pump and second-harmonic mode resonances during all-optical poling. These results unambiguously establish that the photogalvanic effect, responsible for all-optical poling, can overcome phase mismatch constraints, even in resonant systems.

By using the Z-scan method we studied the third-order nonlinear optical parameters of several aminobenziliden-1,3-indandione (ABI) derivatives that have previously been shown to own second-order nonlinear optical properties. Measurements were carried out using two 1064 nm Nd:YAG lasers with picosecond (ps) and nanosecond (ns) pulse widths, respectively. When ns laser was employed in the Z-scan setup, a strong thermal lensing took place resulting in severe overestimation of optical Kerr coefficients. Due to this reason the ps laser was employed to evaluate correct magnitude of Kerr effect. For investigated organic molecules, experimental results show that two-photon absorption at 1064 nm is in correlation with molar extinction coefficient at 532 nm. Here we demonstrate good linear correlation between values of second-order molecular hyperpolarizability determined experimentally and those obtained by quantum chemical modeling.

The coherent photogalvanic effect leads to the generation of a current under the absorption interference of coherent beams and allows for the inscription of space‐charge gratings leading to a second‐order susceptibility (χ(2)). The inscribed grating automatically results in quasi‐phase‐matching between the interfering beams. Theoretical and experimental studies, considering the degenerate case of second‐harmonic generation, show significant conversion efficiency enhancements. However, the link between the theory and experiment is not fully established such that general guidelines and achievable conversion efficiency for a given material platform are still unclear. In this work, the phenomenological model of coherent photogalvanic effect in optical waveguides is theoretically analyzed. This model predicts the existence of non‐degenerate sum‐frequency generation quasi‐phase‐matching gratings, which is confirmed experimentally for the first time. Furthermore, the time dynamics of the space‐charge grating inscription in coherent photogalvanic process is formulated. Based on the developed theoretical equations, the material parameters governing the process for stoichiometric silicon nitride are extracted. The results obtained provide a basis to compare the performances and potentials of different platforms. This work not only supplements the theory of coherent photogalvanic effect, but also enables us to identify critical parameters and limiting factors for the inscription of χ(2) gratings.

In this paper we describe the principles of operation as well as the fabrication and testing steps of an all-organic waveguide modulator. The modulator comprises an SU-8 core and an electro-optic host-guest polymer cladding. The polymer properties are tuned in order to achieve single mode operation. We used direct-write laser lithography in two steps for the preparation of the devices. The electro-optic coefficient of the polymer is estimated from observing the modulation of the device operated in push-pull mode.