<p>We report a large third-order nonlinear optical response of palladium diselenide (PdSe₂) films – a two-dimensional (2D) noble metal dichalcogenide material. Both open-aperture (OA) and closed-aperture (CA) Z-scan measurements are performed with a femtosecond pulsed laser at 800 nm to investigate the nonlinear absorption and nonlinear refraction, respectively. In the OA experiment, we observe optical limiting behaviour originating from large two photo absorption (TPA) in the PdSe₂ film of <i>β =</i> 3.26 × 10^-8 m/W. In the CA experiment, we measure a peak-valley response corresponding to a large and negative Kerr nonlinearity of <i>n</i>₂ = -1.33×10^-15 m²/W – two orders of magnitude larger than bulk silicon. We also characterize the variation of <i>n</i>₂ as a function of laser intensity, observing that <i>n</i>₂ decreases in magnitude with incident laser intensity, becoming saturated at <i>n</i>₂ = -9.96×10^-16 m²/W at high intensities. These results verify the large third-order nonlinear optical response of 2D PdSe₂ as well as its strong potential for high performance nonlinear photonic devices.</p>

Layered two-dimensional (2D) graphene oxide (GO) films are integrated with micro-ring resonators (MRRs) to experimentally demonstrate enhanced nonlinear optics in the form of four-wave mixing (FWM). Both uniformly coated and patterned GO films are integrated on CMOS-compatible doped silica MRRs using a large-area, transfer-free, layer-by-layer GO coating method together with photolithography and lift-off processes, yielding precise control of the film thickness, placement, and coating length. The high Kerr nonlinearity and low loss of the GO films combined with the strong light-matter interaction within the MRRs results in a significant improvement in the FWM efficiency in the hybrid MRRs. Detailed FWM measurements are performed at different pump powers and resonant wavelengths for the uniformly coated MRRs with 1−5 layers of GO as well as the patterned devices with 10−50 layers of GO. The experimental results show good agreement with theory, achieving up to ~7.6-dB enhancement in the FWM conversion efficiency (CE) for an MRR uniformly coated with 1 layer of GO and ~10.3-dB for a patterned device with 50 layers of GO. By fitting the measured CE as a function of pump power for devices with different numbers of GO layers, we also extract the dependence of GO’s third-order nonlinearity on layer number and pump power, revealing interesting physical insights about the evolution of the layered GO films from 2D monolayers to quasi bulk-like behavior. These results confirm the high nonlinear optical performance of integrated photonic resonators incorporated with 2D layered GO films.

Layered two-dimensional (2D) GO films are integrated with silicon-on-insulator (SOI) nanowire waveguides to experimentally demonstrate an enhanced Kerr nonlinearity, observed through self-phase modulation (SPM). The GO films are integrated with SOI nanowires using a large-area, transfer-free, layer-by-layer coating method that yields precise control of the film thickness. The film placement and coating length are controlled by opening windows in the silica cladding of the SOI nanowires. Owing to the strong mode overlap between the SOI nanowires and the highly nonlinear GO films, the Kerr nonlinearity of the hybrid waveguides is significantly enhanced. Detailed SPM measurements using picosecond optical pulses show significant spectral broadening enhancement for SOI nanowires coated with 2.2-mm-long films of 1−3 layers of GO, and 0.4-mm-long films with 5−20 layers of GO. By fitting the experimental results with theory, the dependence of GO’s <i>n</i>₂ on layer number and pulse energy is obtained, showing interesting physical insights and trends of the layered GO films from 2D monolayers to quasi bulk-like behavior. Finally, we show that by coating SOI nanowires with GO films the effective nonlinear parameter of SOI nanowires is increased 16 fold, with the effective nonlinear figure of merit (FOM) increasing by about 20 times to FOM > 5. These results reveal the strong potential of using layered GO films to improve the Kerr nonlinear optical performance of silicon photonic devices.

<p>Polarization selective devices, such as polarizers and polarization selective resonant cavities (e.g., gratings and ring resonators), are core components for polarization control in optical systems and find wide applications in polarization-division-multiplexing, coherent optical detection, photography, liquid crystal display, and optical sensing. In this paper, we demonstrate integrated waveguide polarizers and polarization-selective micro-ring resonators (MRRs) incorporated with graphene oxide (GO). We achieve highly precise control of the placement, thickness, and length of the GO films coated on integrated photonic devices by using a solution-based, transfer-free, and layer-by-layer GO coating method followed by photolithography and lift-off processes. The latter overcomes the layer transfer fabrication limitations of 2D materials and represent a significant advance towards manufacturing integrated photonic devices incorporated with 2D materials. We measure the performance of the waveguide polarizer for different GO film thicknesses and lengths versus polarization, wavelength, and power, achieving a very high polarization dependent loss (PDL) of ~ 53.8 dB. For GO-coated integrated MRRs, we achieve an 8.3-dB polarization extinction ratio between the TE and TM resonances, with the extracted propagation loss showing good agreement with the waveguide results. Furthermore, we present layer-by-layer characterization of the linear optical properties of 2D layered GO films, including detailed measurements that conclusively determine the material loss anisotropy of the GO films as well as the relative contribution of film loss anisotropy versus polarization-dependent mode overlap, to the device performance. These results offer interesting physical insights and trends of the layered GO films from monolayer to quasi bulk like behavior and confirm the high-performance of integrated polarization selective devices incorporated with GO films.</p>