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Photonic integrated circuits with second-order (χ⁽²⁾) nonlinearities are rapidly scaling to remarkably low powers. At this time, state-of-the-art devices achieve saturated nonlinear interactions with thousands of photons when driven by continuous-wave lasers, and further reductions in these energy requirements enabled by the use of ultrafast pulses may soon push nonlinear optics into the realm of single-photon nonlinearities. This tutorial reviews these recent developments in ultrafast nonlinear photonics, discusses design strategies for realizing few-photon nonlinear interactions, and presents a unified treatment of ultrafast quantum nonlinear optics using a framework that smoothly interpolates from classical behaviors to the few-photon scale. These emerging platforms for quantum optics fundamentally differ from typical realizations in cavity quantum electrodynamics due to the large number of coupled optical modes. Classically, multimode behaviors have been well studied in nonlinear optics, with famous examples including soliton formation and supercontinuum generation. In contrast, multimode quantum systems exhibit a far greater variety of behaviors, and yet closed-form solutions are even sparser than their classical counterparts. In developing a framework for ultrafast quantum optics, we identify what behaviors carry over from classical to quantum devices, what intuition must be abandoned, and what new opportunities exist at the intersection of ultrafast and quantum nonlinear optics. Although this article focuses on establishing connections between the classical and quantum behaviors of devices withχ⁽²⁾nonlinearities, the frameworks developed here are general and are readily extended to the description of dynamical processes based on third-orderχ⁽³⁾nonlinearities. 

Numerical modeling of ultrashort pulse propagation is important for designing and understanding the underlying dynamical processes in devices that take advantage of highly nonlinear interactions in dispersion-engineered optical waveguides. Once the spectral bandwidth reaches an octave or more, multiple types of nonlinear polarization terms can drive individual optical frequencies. This issue is particularly prominent inχ⁽²⁾devices where all harmonics of the input pulse are generated and there can be extensive spectral overlap between them. Single-envelope approaches to pulse propagation have been developed to address these complexities; this has led to a significant mismatch between the strategies used to analyze moderate-bandwidth devices (usually involving multi-envelope models) and those used to analyze octave-spanning devices (usually involving models with one envelope per waveguide mode). Here we unify the different strategies by developing a common framework, applicable to any optical bandwidth, that allows for a side-by-side comparison between single- and multi-envelope models. We include bothχ⁽²⁾andχ⁽³⁾interactions in these models, with emphasis onχ⁽²⁾interactions. We show a detailed example based on recent supercontinuum generation experiments in a thin-film LiNbO₃on sapphire quasi-phase-matching waveguide. Our simulations of this device show good agreement between single- and multi-envelope models in terms of the frequency comb properties of the electric field, even for multi-octave-spanning spectra. Building on this finding, we explore how the multi-envelope approach can be used to develop reduced models that help build physical insights about new ultrafast photonics devices enabled by modern dispersion-engineered waveguides, and discuss practical considerations for the choice of such models. More broadly, we give guidelines on the pros and cons of the different modeling strategies in the context of device design, numerical efficiency, and accuracy of the simulations. 

Over the last few decades, nonlinear optics has become significantly more nonlinear, traversing nearly a billionfold improvement in energy efficiency, with ultrafast nonlinear nanophotonics in particular emerging as a frontier for combining both spatial and temporal engineering. At present, cutting-edge experiments in nonlinear nanophotonics place us just above themesoscopicregime, where a few hundred photons suffice to trigger highly nonlinear dynamics. In contrast to classical or deep-quantum optics, the mesoscale is characterized by dynamical interactions between mean-field, Gaussian, and non-Gaussian quantum features, all within a close hierarchy of scales. When combined with the inherent multimode complexity of optical fields, such hybrid quantum-classical dynamics present theoretical, experimental, and engineering challenges to the contemporary framework of quantum optics. In this review, we highlight the unique physics that emerges in multimode nonlinear optics at the mesoscale and outline key principles for exploiting both classical and quantum features to engineer novel functionalities. We briefly survey the experimental landscape and draw attention to outstanding technical challenges in materials, dispersion engineering, and device design for accessing mesoscopic operation. Finally, we speculate on how these capabilities might usher in some new paradigms in quantum photonics, from quantum-augmented information processing to nonclassical-light-driven dynamics and phenomena to all-optical non-Gaussian measurement and sensing. The physics unlocked at the mesoscale present significant challenges and opportunities in theory and experiment alike, and this review is intended to serve as a guide to navigating this new frontier in ultrafast quantum nonlinear optics. 

We propose a new approach to supercontinuum generation and carrier-envelope-offset detection based on saturated second-order nonlinear interactions in dispersion-engineered nanowaveguides. The technique developed here broadens the interacting harmonics by forming stable bifurcations of the pulse envelopes due to an interplay between phase-mismatch and pump depletion. We first present an intuitive heuristic model for spectral broadening by second-harmonic generation of femtosecond pulses and show that this model agrees well with experiments. Then, having established strong agreement between theory and experiment, we develop scaling laws that determine the energy required to generate an octave of bandwidth as a function of input pulse duration, device length, and input pulse chirp. These scaling laws suggest that future realization based on this approach could enable supercontinuum generation with orders of magnitude less energy than current state-of-the-art devices. 

The sensitivity of gravitational-wave detectors is limited by the mechanical loss associated with the amorphous coatings of the detectors’ mirrors. Amorphous silicon has higher refraction index and lower mechanical loss than current high-index coatings, but its optical absorption at the wavelength used for the detectors is at present large. The addition of hydrogen to the amorphous silicon network reduces both optical absorption and mechanical loss for films prepared under a range of conditions at all measured wavelengths and temperatures, with a particularly large effect on films grown at room temperature. The uptake of hydrogen is greatest in the films grown at room temperature, but still below 1.5 at.% H, which show an ultralow optical absorption (below 10 ppm) measured at 2000 nm for 500-nm-thick films. These results show that hydrogenation is a promising strategy to reduce both optical absorption and mechanical loss in amorphous silicon, and may enable fabrication of mirror coatings for gravitational-wave detectors with improved sensitivity. 

The ability to observe astronomical events through the detection of gravitational waves relies on the quality of multilayer coatings used on the optical mirrors of interferometers. Amorphous Ta2O5 (including TiO2:Ta2O5) currently limits detector sensitivity due to high mechanical loss. In this paper, mechanical loss measured at both cryogenic and room temperatures of amorphous Ta2O5 films grown by magnetron sputtering and annealed in air at 500 ◦C is shown to decrease for elevated growth temperature. Films grown at 310 ◦C and annealed yield a mechanical loss of 3.1×10−4 at room temperature, the lowest value reported for pure amorphous Ta2O5 grown by magnetron sputtering to date, and comparable to the lowest values obtained for films grown by ion beam sputtering. Additionally, the refractive index n increases 6% for elevated growth temperature, which could lead to improved sensitivity of gravitational-wave detectors by allowing a thickness reduction in the mirrors’ coatings. Structural characterization suggests that the observed mechanical loss reduction in amorphous Ta2O5 films with increasing growth temperature correlates with a reduction in the coordination number between oxygen and tantalum atoms, consistent with TaOx polyhedra with increased corner-sharing and reduced edge- and facesharing structures. 

Brownian thermal noise as a result of mechanical loss in optical coatings will become the dominant source of noise at the most sensitive frequencies of ground-based gravitational-wave detectors. Experiments found, however, that a candidate material, amorphous Ta2O5, is unable to form an ultrastable glass and, consequently, to yield a film with significantly reduced mechanical loss through elevated-temperature deposition alone. X-ray scattering PDF measurements are carried out on films deposited and subsequently annealed at various temperatures. Inverse atomic modeling is used to analyze the short and medium range features in the atomic structure of these films. Furthermore, in silico deposition simulations of Ta2O5 are carried out at various substrate temperatures and an atomic level analysis of the growth at high temperatures is presented. It is observed that upon elevated-temperature deposition, short range features remain identical, whereas medium range order increases. After annealing, however, both the short and medium range orders of films deposited at different substrate temperatures are nearly identical. A discussion on the surface diffusion and glass transition temperatures indicates that future pursuits of ultrastable low-mechanical-loss films through elevated temperature deposition should focus on materials with a high surface mobility, and/or lower glass transition temperatures in the range of achievable deposition temperatueres. 

Silicon is a common material for photonics due to its favorable optical properties in the telecom and mid-wave IR bands, as well as compatibility with a wide range of complementary metal–oxide semiconductor (CMOS) foundry processes. Crystalline inversion symmetry precludes silicon from natively exhibiting second-order nonlinear optical processes. In this work, we build on recent works in silicon photonics that break this material symmetry using large bias fields, thereby enabling χ (2) interactions. Using this approach, we demonstrate both second-harmonic generation (with a normalized efficiency of 0.20%W −1 cm −2 ) and, to our knowledge, the first degenerate χ (2) optical parametric amplifier (with an estimated normalized gain of 0.6dBW −1/2 cm −1 ) using silicon-on-insulator waveguides fabricated in a CMOS-compatible commercial foundry. We expect this technology to enable the integration of novel nonlinear optical devices such as optical parametric amplifiers, oscillators, and frequency converters into large-scale, hybrid photonic–electronic systems by leveraging the extensive ecosystem of CMOS fabrication. 

Abstract This article reviews recent progress in quasi-phasematched χ ( 2 ) nonlinear nanophotonics, with a particular focus on dispersion-engineered nonlinear interactions. Throughout this article, we establish design rules for the bandwidth and interaction lengths of various nonlinear processes, and provide examples for how these processes can be engineered in nanophotonic devices. In particular, we apply these rules towards the design of sources of non-classical light and show that dispersion-engineered devices can outperform their conventional counterparts. Examples include ultra-broadband optical parametric amplification as a resource for measurement-based quantum computation, dispersion-engineered spontaneous parametric downconversion as a source of separable biphotons, and synchronously pumped nonlinear resonators as a potential route towards single-photon nonlinearities.