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 β = 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 n₂ = -1.33×10^-15 m²/W – two orders of magnitude larger than bulk silicon. We also characterize the variation of n₂ as a function of laser intensity, observing that n₂ decreases in magnitude with incident laser intensity, becoming saturated at n₂ = -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.

The Kerr nonlinear optical performance of silicon nanowire waveguides integrated with 2D layered graphene oxide (GO) films is theoretically studied and optimized based on experimentally measured linear and nonlinear optical parameters of the GO films. The strong mode overlap between the silicon nanowires and highly nonlinear GO films yields a significantly enhanced Kerr nonlinearity for the hybrid waveguides. A detailed analysis for the influence of waveguide geometry and GO film thickness on the propagation loss, nonlinear parameter, and nonlinear figure of merit (FOM) is performed. The results show that the effective nonlinear parameter and nonlinear FOM can be increased by up to ≈52 and ≈79 times relative to bare silicon nanowires, respectively. Self-phase modulation (SPM)-induced spectral broadening of optical pulses is used as a benchmark to evaluate the nonlinear performance, examining the trade-off between enhancing Kerr nonlinearity and minimizing loss. By optimizing the device parameters to balance this, a high spectral broadening factor of 27.6 can be achieved ‒ more than 6 times that achieved in previous experiments. Finally, the influence of pulse chirp, material anisotropy, and the interplay between saturable absorption and SPM is also discussed. These results provide useful guidance for optimizing the Kerr nonlinear optical performance of silicon waveguides integrated with 2D layered GO films.

With superior optical properties, high flexibility in engineering its material properties, and strong capability for large-scale on-chip integration, graphene oxide (GO) is an attractive solution for on-chip integration of two-dimensional (2D) materials to implement functional integrated photonic devices capable of new features. Over the past decade, integrated GO photonics, representing an innovative merging of integrated photonic devices and thin GO films, has experienced significant development, leading to a surge in many applications covering almost every field of optical sciences. This paper reviews the recent advances in this emerging field, providing an overview of the optical properties of GO as well as methods for the on-chip integration of GO. The main achievements made in GO hybrid integrated photonic devices for diverse applications are summarized. The open challenges as well as the potential for future improvement are also discussed.

We experimentally demonstrate enhanced spectral broadening of femtosecond optical pulses after propagation through silicon-on-insulator (SOI) nanowire waveguides integrated with two-dimensional (2D) graphene oxide (GO) films. Owing to the strong mode overlap between the SOI nanowires and the GO films with a high Kerr nonlinearity, the self-phase modulation (SPM) process in the hybrid waveguides is significantly enhanced, resulting in greatly improved spectral broadening of the femtosecond optical pulses. A solution-based, transfer-free coating method is used to integrate GO films onto the SOI nanowires with precise control of the film thickness. Detailed SPM measurements using femtosecond optical pulses are carried out, achieving a broadening factor of up to ~4.3 for a device with 0.4-mm-long, 2 layers of GO. By fitting the experimental results with theory, we obtain an improvement in the waveguide nonlinear parameter by a factor of ~3.5 and the effective nonlinear figure of merit (FOM) by a factor of ~3.8, relative to the uncoated waveguide. Finally, we discuss the influence of GO film length on the spectral broadening and compare the nonlinear optical performance of different integrated waveguides coated with GO films. These results confirm the improved nonlinear optical performance for silicon devices integrated with 2D GO films.

We theoretically investigate and optimize four-wave mixing (FWM) in silicon nitride (SiN) waveguides integrated with two-dimensional (2D) layered graphene oxide (GO) films. Based on extensive previous measurements of the material parameters of the GO films, we perform detailed analysis for the influence of device parameters including waveguide geometry, GO film thickness, length, and coating position on the FWM conversion efficiency (CE) and conversion bandwidth (CB). The influence of dispersion and photo-thermal changes in the GO films is also discussed. Owing to the strong mode overlap between the SiN waveguides and the highly nonlinear GO films, FWM in the hybrid waveguides can be significantly enhanced. We obtain good agreement with previous experimental results and show that by optimizing the device parameters to balance the trade-off between Kerr nonlinearity and loss, the FWM CE can be improved by as much as ~20.7 dB and the FWM CB can be increased by ~4.4 folds, relative to the uncoated waveguides. These results highlight the significantly enhanced FWM performance that can be achieved in SiN waveguides by integrating 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 n₂ 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.

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.