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Lithium niobate is a promising material for developing quantum acoustic technologies due to its strong piezoelectric effect and availability in the form of crystalline thin films of high quality. However, at radio frequencies and cryogenic temperatures, these resonators are limited by the presence of decoherence and dephasing due to two-level systems. To mitigate these losses and increase device performance, a more detailed picture of the microscopic nature of these loss channels is needed. In this study, we fabricate several lithium niobate acoustic wave resonators and apply different processing steps that modify their surfaces. These treatments include argon ion sputtering, annealing, and acid cleans. We characterize the effects of these treatments using three surface-sensitive measurements: cryogenic microwave spectroscopy measuring density and coupling of TLS to mechanics, X-ray photoelectron spectroscopy and atomic force microscopy. We learn from these studies that, surprisingly, increases of TLS density may accompany apparent improvements in the surface quality as probed by the latter two approaches. Our work outlines the importance that surfaces and fabrication techniques play in altering acoustic resonator coherence, and suggests gaps in our understanding as well as approaches to address them.

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.

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.

Optical parametric amplification is one of the most flexible approaches for generating coherent light at long wavelengths, but typical implementations require prohibitively large pump pulse energies to realize useful amounts of gain. In this work, we experimentally demonstrate an approach to optical parametric amplification in which an interplay between parametric gain and symmetric temporal walk-off confines the non-degenerate signal and idler to form a three-wave soliton. Gain-trapped solitons propagate stably over arbitrarily long interaction lengths, which reduces the energy required for high-gain operation by orders of magnitude. The devices demonstrated here realize large parametric gains (>70dB) with only picojoules of pump pulse energy in a 5-mm-long thin-film lithium niobate on sapphire nanowaveguide. In addition, we observe an array of desirable features including high conversion efficiencies (>50%), wide tuning ranges (>100nm), and broad spectral bandwidths (>180nm 3 dB for the 3200-nm idler). When combined with the dispersion engineering available in tightly confining nanowaveguides, this approach enables high-gain optical parametric amplifiers operating at any wavelength.

Mid-infrared spectroscopy, an important technique for sensing molecules, has encountered barriers from sources either limited in tuning range or excessively bulky for widespread use. We present a compact, efficient, and broadly tunable optical parametric oscillator surmounting these challenges. Leveraging dispersion-engineered thin-film lithium niobate-on-sapphire photonics and a singly resonant cavity allows broad, controlled tuning over an octave from 1.5–3.3 µm. The device generates >25mW of mid-infrared light at 3.2 µm with 15% conversion efficiency. The ability to precisely control the device’s mid-infrared emission enables spectroscopy of methane and ammonia, demonstrating our approach’s relevance for sensing. Our work signifies an important advance in nonlinear photonics miniaturization, bringing practical field applications of high-speed, broadband mid-infrared spectroscopy closer to reality.

Synchronously pumped optical parametric oscillators (OPOs) are highly efficient sources of long-wavelength pulses and nonclassical light, making them invaluable for applications in spectroscopy, metrology, multi-photon microscopy, and quantum computation. Typical systems based on free-space cavities either operate non-degenerately, which limits their efficiency, or use active feedback control to achieve degenerate operation, which limits these systems to dedicated low-noise environments. In this work, we demonstrate a femtosecond monolithically integrated OPO. In contrast with bulk OPOs, our monolithic 10 GHz cavity, based on reverse-proton-exchanged lithium niobate, operates stably without active locking. By detuning the repetition rate of the free-running pump laser from the cavity free spectral range, we control the intracavity pulse dynamics and observe many of the operating regimes previously encountered in free-space degenerate OPOs, such as box-pulsing and quadratic bright-dark solitons (simultons), in addition to non-degenerate operation. When operated in the simulton regime and pumped with 125 fs pulses at 1 µm, this monolithic OPO chip outputs broadband sech²pulses (63 nm, 3 dB) with tens of milliwatts of average power.

The realization of deterministic photon–photon gates is a central goal in optical quantum computation and engineering. A longstanding challenge is that optical nonlinearities in scalable, room-temperature material platforms are too weak to achieve the required strong coupling, due to the critical loss-confinement trade-off in existing photonic structures. In this work, we introduce a spatio-temporal confinement method, dispersion-engineered temporal trapping, to circumvent the trade-off, enabling a route to all-optical strong coupling. Temporal confinement is imposed by an auxiliary trap pulse via cross-phase modulation, which, combined with the spatial confinement of a waveguide, creates a “flying cavity” that enhances the nonlinear interaction strength by at least an order of magnitude. Numerical simulations confirm that temporal trapping confines the multimode nonlinear dynamics to a single-mode subspace, enabling high-fidelity deterministic quantum gate operations. With realistic dispersion engineering and loss figures, we show that temporally trapped ultrashort pulses could achieve strong coupling on near-term nonlinear nanophotonic platforms. Our results highlight the potential of ultrafast nonlinear optics to become the first scalable, high-bandwidth, and room-temperature platform that achieves strong coupling, opening a path to quantum computing, simulation, and light sources.

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 enablingχ⁽²⁾interactions. Using this approach, we demonstrate both second-harmonic generation (with a normalized efficiency of 0.20%W⁻¹cm⁻²) and, to our knowledge, the first degenerateχ⁽²⁾optical parametric amplifier (with an estimated normalized gain of 0.6dBW^−1/2cm⁻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.