Enhanced Self‐Phase Modulation in Silicon Nitride Waveguides Integrated With 2D MoS 2 Films

Self-phase modulation (SPM) is an important third-order nonlinear optical process that has been widely used in many applications, such as broadband optical sources, optical diodes, optical spectroscopy, pulse compression, and many others. The ability to realize SPM based on-chip integrated photonic devices will reap attractive benefits of compact footprint, high stability, high scalability, and low-cost mass production. Here, we experimentally investigate enhanced SPM in silicon nitride (Si3N4) waveguides by integrating with 2D graphene oxide (GO) films. The on-chip integration of GO films is achieved on Si3N4 waveguides through a solution-based, transfer-free, layer-by-layer coating method with precise control of the film thickness. We use both picosecond and femtosecond optical pulses to perform detailed SPM measurements. Owing to the high Kerr nonlinearity of GO, the GO-coated waveguides show significantly improved spectral broadening for both the picosecond and femtosecond optical pulses compared to the uncoated waveguide, achieving a broadening factor of up to ~3.4 for a device with 2 layers of GO. Based on the experimental results which show good agreement with theory, we obtain an improvement in the waveguide nonlinear parameter by a factor of up to 18.4 and a Kerr coefficient (n2) of GO that is about 5 orders of magnitude higher than Si3N4. These results reveal the effectiveness of 2D GO films to improve the nonlinear performance of Si3N4 waveguides.

Silicon nitride (SiN) waveguides with ultra-low optical loss enable integrated photonic applications including low noise, narrow linewidth lasers, chip-scale nonlinear photonics, and microwave photonics. Lasers are key components to SiN photonic integrated circuits (PICs), but are difficult to fully integrate with low-index SiN waveguides due to their large mismatch with the high-index III-V gain materials. The recent demonstration of multilayer heterogeneous integration provides a practical solution and enabled the first-generation of lasers fully integrated with SiN waveguides. However, a laser with high device yield and high output power at telecommunication wavelengths, where photonics applications are clustered, is still missing, hindered by large mode transition loss, non-optimized cavity design, and a complicated fabrication process. Here, we report high-performance lasers on SiN with tens of milliwatts output power through the SiN waveguide and sub-kHz fundamental linewidth, addressing all the aforementioned issues. We also show Hertz-level fundamental linewidth lasers are achievable with the developed integration techniques. These lasers, together with high-Q SiN resonators, mark a milestone towards a fully integrated low-noise silicon nitride photonics platform. This laser should find potential applications in LIDAR, microwave photonics and coherent optical communications.

We experimentally demonstrate enhanced self-phase modulation (SPM) in silicon nitride (Si3N4) waveguides integrated with 2D graphene oxide (GO) films. GO films are integrated onto Si3N4 waveguides using a solution-based, transfer-free coating method that enables precise control of the film thickness. Detailed SPM measurements are carried out using both picosecond and femtosecond optical pulses. Owing to the high Kerr nonlinearity of GO, the hybrid waveguides show significantly improved spectral broadening compared to the uncoated waveguide, achieving a broadening factor of up to ~3.4 for a device with 2 layers of GO. By fitting the experimental results with theory, we obtain an improvement in the waveguide nonlinear parameter by a factor of up to 18.4 and a Kerr coefficient (n2) of GO that is about 5 orders of magnitude higher than Si3N4. Finally, we provide a theoretical analysis for the influence of GO film length, coating position, and its saturable absorption on the SPM performance. These results verify the effectiveness of on-chip integrating 2D GO films to enhance the nonlinear optical performance of Si3N4 devices.

Mid-infrared (mid-IR) sensors consisting of silicon nitride (SiN) waveguides were designed and tested to detect volatile organic compounds (VOCs). SiN thin films, prepared by low-pressure chemical vapor deposition (LPCVD), have a broad mid-IR transparent region and a lower refractive index (nSiN = 2.0) than conventional materials such as Si (nSi = 3.4), which leads to a stronger evanescent wave and therefore higher sensitivity, as confirmed by a finite-difference eigenmode (FDE) calculation. Further, in-situ monitoring of three VOCs (acetone, ethanol, and isoprene) was experimentally demonstrated through characteristic absorption measurements at wavelengths λ = 3.0–3.6 μm. The SiN waveguide showed a five-fold sensitivity improvement over the Si waveguide due to its stronger evanescent field. To our knowledge, this is the first time SiN waveguides are used to perform on-chip mid-IR spectral measurements for VOC detection. Thus, the developed waveguide sensor has the potential to be used as a compact device module capable of monitoring multiple gaseous analytes for health, agricultural and environmental applications.

We present suspended heater structures fabricated in a standard C- and O-band silicon (Si) photonics platform that can achieve sufficiently high local temperatures to induce effective refractive index trimming of Si and silicon nitride (SiN) waveguides with 30 - 90 mW of applied electrical power. Following thermal trimming at moderate powers (≤40 mW), maximum changes in the averaged waveguide effective refractive index of -5.18 × 10-3 and -7.9 × 10-4 are demonstrated in SiN and Si waveguides, respectively, at a wavelength of 1550 nm. At higher powers, SiN waveguides exhibit positive averaged effective index changes up to ≈0.02, demonstrating bi-directional index trimming. As an example application, we demonstrate bias point trimming of a carrier injection Mach-Zehnder switch. Through investigations of the origin of the thermal trimming effect, we hypothesize that changes in the silica (SiO2) waveguide cladding may be a primary underlying mechanism at temperatures ≳300°C, with significant trimming of SiN waveguide cores occurring at larger temperatures ≳510°C. As the trimming experiments represent a form of accelerated thermal aging, we estimate the aging behavior of the suspended heaters by fitting and extrapolating the measured datasets to 100 - 200°C operating temperatures over five years.

We report enhanced nonlinear optics in nanowires, waveguides, and ring resonators by introducing layered two-dimensional (2D) graphene oxide (GO) films through experimental demonstration. The GO films are integrated on silicon-on-insulator nanowires (SOI), high index doped silica glass, and silicon nitride (SiN) waveguides and microring resonators (MRRs), to demonstrate an improved optical nonlinearity including Kerr nonlinearity and four-wave mixing (FWM). By using a large-area, transfer-free, layer-by-layer GO coating method with photolithography and lift-off processes, we integrate GO films on these complementary metal-oxide-semiconductor (CMOS)-compatible devices. For SOI nanowires, significant spectral broadening of optical pulses in GO-coated SOI nanowires induced by self-phase modulation (SPM) is observed, achieving a high spectral broadening factor of 4.34 for a device with a patterned film including 10 layers of GO. A significant enhancement in the nonlinear figure of merit (FOM) for silicon nanowires by a factor of 20 is also achieved, resulting in a FOM > 5. For Hydex and SiN waveguides, enhanced FWM in the GO-coated waveguides is achieved, where conversion efficiency (CE) enhancements of up to 6.9 dB and 9.1 dB relative to the uncoated waveguides. For MRRs, an increase of up to ~10.3 dB in the FWM CE is achieved due to the resonant enhancement effect. These results reveal the strong potential of GO films to improve the nonlinear optics of nanowires, waveguides, and ring resonators.

Layered 2D graphene oxide (GO) films are integrated with silicon nitride (SiN) waveguides to experimentally demonstrate an enhanced Kerr nonlinearity via four‐wave mixing (FWM). SiN waveguides with both uniformly coated and patterned GO films are fabricated based on a transfer‐free, layer‐by‐layer GO coating method along with standard photolithography and lift‐off processes, yielding precise control of the film thickness, placement, and coating length. Detailed FWM measurements are carried out for the fabricated devices with different numbers of GO layers and at different pump powers, achieving up to ≈7.3 dB improvement in the FWM conversion efficiency for an uniformly coated device with one layer of GO and ≈9.1 dB for a patterned device with five layers of GO. A detailed analysis of the influence of pattern length and position on the FWM performance is performed. The dependence of GO's third‐order nonlinearity on layer number and pump power is also extracted, revealing interesting physical insights about the layered 2D GO films. Finally, an enhancement is obtained in the effective nonlinear parameter of the hybrid waveguides by over a factor of 100 relative to bare SiN waveguide. These results demonstrate the high nonlinear optical performance of SiN waveguides integrated with layered 2D GO films.

In this work, we experimentally study the optical Kerr nonlinearities of graphene/Si hybrid waveguides with enhanced self-phase modulation. In the case of CMOS compatible materials for nonlinear optical signal processing, Si and silicon nitride waveguides have been extensively investigated over the past decade. However, Si waveguides exhibit strong two-photon absorption (TPA) at telecommunication wavelengths, which leads to a significant reduction of the nonlinear figure-of-merit (FOM). In contrast, a silicon nitride based material system usually suppresses the TPA but simultaneously leads to the reduction of Kerr nonlinearity by one order of magnitude. Here, we introduce a graphene/Si hybrid waveguide, which maintains the optical properties and CMOS compatibility of Si waveguides, while enhancing the Kerr nonlinearity, by transferring over to the top of the waveguides. The graphene/Si waveguides are measured to have an enhanced nonlinear parameter of 510 W−1 m−1, compared with that of the Si waveguide of 150 W−1 m−1. An enhanced nonlinear FOM of 2.48 ± 0.25 has been achieved, which is four times larger than that of the Si waveguide of 0.6 ± 0.1. This work reveals the potential application of graphene/Si hybrid waveguides with high Kerr nonlinearity and FOM for nonlinear all-optical signal processing.

Towards monolithic low-loss silicon nitride waveguides on a mature 200 mm CMOS platform

In the past decades quantum optics has been at the forefront of quantum innovative technologies. For practical applications, scalable platforms for implementation of quantum optical circuits are vital. This thesis presents two new platforms for scalable implementation of quantum optical circuits, namely, modular approach and monolithic integration. Here, we take the first steps towards the integration of three main elements of every quantum optics circuits: Single-photon emitters, single-photon detectors, and quantum logics. Until now, most quantum optical circuits used separate platforms for single-photon generation and detection. The main challenge in the integration of these technologies, which have different requirements, has slowed down the research in the field. Here, we integrate sources and detectors by first fabricating the devices on their own platform and then transferring and combining them together. Plasma enhanced chemical vapor deposition of silicon nitride followed by etching optical waveguides connect these elements. Removing the Poissonian optical excitation field from the quantum circuit is necessary for integration. Classical optical excitation can be avoided if the sources are electrically pumped. However, fabrication of high-quality electrically pumped sources, suitable for integration, has been limited. The experiments described in chapter 4 are our first step towards addressing the mentioned problem. Defect-free nanowires are grown on l100g direction and their optoelectronic performance are characterized. Nanowire quantum dots, thanks to their waveguiding, purity, coherence and their potentials for deterministic integration with other optical circuits, are promising single-photon sources for on-chip quantum optics. However, precise control of the emission energy of the quantum dots by growth has not become possible yet. Chapter 5 describes a method for on-chip tuning of emission energy of nanowire quantum dots using strain fields. We show the emission energy of independent nanowire quantum dots can be brought into degeneracy without affecting their single-photon emission properties. The quantum optical components have to be routed and connected together to form functional circuits. On a chip, this is usually carried out using optical waveguides. Moreover, manipulation of single photons has to be done in a scalable fashion. Again optical waveguides and ring resonators are very good candidates for this task. Therefore, understanding the behavior of these circuits such as their losses, polarization dependence, and temperature behavior is important. The experiment described in chapter 6 studies the behavior of plasma enhanced silicon nitride waveguides in cryogenic temperatures. We concluded in this chapter that due to weak thermo-optic sensitivity of silicon nitride at cryogenic temperatures, the available thermal budget on the system should be carefully considered. An important step in achieving a scalable platform for quantum optical circuits is deterministic and efficient integration of single-photon sources. In chapter 7, we demonstrate successful integration of III-V nanowire quantum dots with silicon nitride waveguides. The nanowires are deterministically selected and transferred from the original growth chip to the new substrate where they are integrated with low-loss silicon nitride waveguides. Our measurements show that the integrated sources preserve their high quality emission properties. In chapter 8, we describe an alternative approach: amodular method for scalable quantum optics. The proposed technique is based on coupling the single-photon from sources into optical fibers where the photons can be processed and then fed into the single-photon detectors. This approach has high flexibility and is easier to implement but as described in the chapter, at the moment, losses in the interfaces between optical fibers and single-photon sources are a major limiting factor. We conclude the thesis with some possible future directions and exciting new results on integration of single-photon detectors with sources and waveguides. Finally, primary results on on-chip single-photon filtering and removal of the optical excitation field are demonstrated.

The international road map of semiconductors (ITRS) lists 2D materials as possible future materials for electronic devices [ITRS]. Among them, the semiconducting transition metal dichalcogenides (TMDC) like MoS2 or WS2 are the most promising ones. As the miniaturization of electronic devices continues and the sub-5 nm gate limit is reached, direct source-to-drain tunneling will become a problem in Si devices with conventional architecture. 2D TMDC as channel material for FET might overcome this issue in digital CMOS. The larger carrier effective masses of most TMDC result in reduced direct source-to-drain tunneling, while they also yield a large density of states and hence an increased ballistic current in this extreme dimensions [Fiori]. Additionally, the lower in-plane dielectric constants of TMDC enable a better vertical electrostatic control over the channel [Desai]. Still, TMDC will have to compete against other approaches, e.g. multiple-gate transistors [Schwiertz]. Beyond that, other properties of TMDC turn them interesting for future devices, such as their strong absorbance across the visible spectrum for optoelectronic devices [Lotsch]. The first photodetectors, electromluminescent p-n diodes and photovoltaic cells have already been shown [Lopez, Cheng, Tsai]. The excellent mechanical properties additionally enable the realization of different kinds of flexible devices [Schwiertz]. And last but not least, the integration of 2D materials into conventional 3D semiconductor concepts would be another application. For example, the strain originating from the large difference in lattice constants in a 3D heterostructure is often a challenge. Inserting 2D materials might be a solution. Due to the fully terminated surface of a TMDC monolayer, the binding to another material is of van-der-Waals type. Hence, TMDC can be stacked with materials with huge differences in lattice constants without leading to considerable strain or to interface trap densities [Vogel]. First devices with a combination of 2D and 3D materials have already been investigated [Krishna, Lee]. Large-scale fabrication of TMDC is still a challenge to be overcome. Up to now, the most frequently used techniques are either exfoliation of natural layered crystals or the growth via chemical vapor deposition (CVD). Exfoliation is a very time-consuming process with relatively low yield and reproducibility. In CVD, different gaseous precursors decompose on a substrate and react with each other. Thermally evaporated MoO3 and S are commonly used as precursors for the fabrication of MoS2 monolayers via CVD. This technique allows the deposition of monolayered crystallites with a size in the range of micrometers [Dumcenco]. The process is carried out in small experimental reactors, and a uniform deposition on a whole wafer is very challenging. The use of metalorganic precursors is one possibility to enter an industrial scale of fabrication. The development of III/V and II/VI semiconductors has shown that metalorganic chemical vapor deposition (MOCVD) makes controllable and reproducible processes feasible, which are easily scalable and hence suitable for large-area deposition. Additionally, the reactors are well-developed, and a future integration of 2D materials and other semiconductors is within reach. First publications show very good results on the deposition of MoS2 and WSe2 via MOCVD [Kang, Eichfeld]. But despite these works and first simulations of the growth kinetics [Nie], little is known about the growth mechanism. For this reason, we have started to investigate the deposition of 2D MoS2 on an AIXTRON MOCVD reactor.The experiments are carried out in a horizontal hot-wall MOCVD reactor in a 10 × 2 inch configuration. Molybdenum hexacarbonyl (MCO) and Di-tert-butyl sulfide (DTBS) are used as Mo and S sources, respectively. In preliminary experiments, the carrier gas based transport of the precursors into the reactor and possible growth conditions are tested. Their results are used to develop an initial growth process. This process leads to a uniform, wafer-scale deposition of MoS2 on various substrate types such as sapphire (0001), Si (111), and AlN and GaN templates on sapphire substrates. The deposited films mainly consists of MoS2 bilayers and exhibit a very high initial nucleation density. Further investigations of the influence of the growth temperature, the carrier gas composition and the pretreatment of the substrates are carried out. With optimization of these growth parameters, a crystal growth process closer to thermodynamical equilibrium can be achieved. This results in the formation of triangular crystals on sapphire substrates which are also reported from CVD processes and exhibit higher crystal quality [Dumcenco]. Additional experiments are conducted to investigate the nucleation of the films and to further tune nucleation density and lateral growth rate in order to deposit wafer-scale monolayered MoS2 films.

Optical parametric oscillators (OPOs) are ubiquitous sources for efficient frequency conversion and have evolved into robust fiber technology [1] . However, integrated waveguides offer in contrast to photonic crystal fibers a higher nonlinearity resulting in lower necessary pump energies and shorter interaction lengths [2] . Therefore, OPOs would require smaller footprints on a chip with additionally improved stability [3] . Here, we present a waveguide-based OPO (WOPO) exploiting four-wave mixing (FWM) in silicon nitride (Si 3 N 4 ) waveguides, with the potential to be fully integrated.

Patterning of transition metal dichalcogenides catalyzed by surface plasmons with atomic precision

Silicon nitride (Si3N4) waveguides represent a novel photonic platform that is ideally suited for energy efficient and ultrabroadband nonlinear interactions from the visible to the mid-infrared. Chip-based supercontinuum generation in Si3N4 offers a path towards a fully-integrated and highly compact comb source for sensing and time-and-frequency metrology applications. We demonstrate the first successful frequency comb offset stabilization that utilizes a Si3N4 waveguide for octave-spanning supercontinuum generation and achieve the lowest integrated residual phase noise of any diode-pumped gigahertz laser comb to date. In addition, we perform a direct comparison to a standard silica photonic crystal fiber (PCF) using the same ultrafast solid-state laser oscillator operating at 1 µm. We identify the minimal role of Raman scattering in Si3N4 as a key benefit that allows to overcome the fundamental limitations of silica fibers set by Raman-induced self-frequency shift.

A post‐fabrication method is demonstrated that enables spatially deterministic integration of hexagonal boron nitride (hBN) single‐photon emitters onto silicon nitride (SiN) waveguides. Mechanically exfoliated hBN flakes are dry‐transferred onto pre‐fabricated SiN waveguides, and localized femtosecond laser irradiation is employed to induce defects with sub‐microscale spatial precision. Confocal photoluminescence mapping reveals multiple laser‐written bright defects, among which one emitter exhibits narrow spectral linewidth and polarization dependence characteristic of a dipole emitter. The emitter exhibits high brightness and temporal stability, and second‐order photon correlation measurements confirm its single‐photon nature. Furthermore, on‐chip excitation via the SiN waveguide is successfully achieved, demonstrating the compatibility of the approach with mature photonic platform technologies. This deterministic integration technique offers a scalable pathway for incorporating quantum emitters into photonic circuits, paving the way for the development of quantum information processing and communication systems with 2D material hybrid photonic devices.