Optical-parametric-amplification-enhanced background-free spectroscopy.

Traditional absorption spectroscopy has a fundamental difficulty in resolving small absorbance from a strong background due to the instability of laser sources. Existing background-free methods in broadband vibrational spectroscopy help to alleviate this problem but face challenges in realizing either low extinction ratios or time-resolved field measurements. Here, we introduce optical-parametric-amplification-enhanced background-free spectroscopy, in which the excitation background is first suppressed by an interferometer, and then the free-induction decay that carries molecular signatures is selectively amplified. We show that this method can improve the limit of detection in linear interferometry by order(s) of magnitude without requiring lower extinction ratios or a time-resolved measurement, which can benefit sensing applications in detecting trace species.

Ultrafast mode-locked laser in nanophotonic lithium niobate.

Mode-locked lasers (MLLs) generate ultrashort pulses with peak powers substantially exceeding their average powers. However, integrated MLLs that drive ultrafast nanophotonic circuits have remained elusive because of their typically low peak powers, lack of controllability, and challenges when integrating with nanophotonic platforms. In this work, we demonstrate an electrically pumped actively MLL in nanophotonic lithium niobate based on its hybrid integration with a III-V semiconductor optical amplifier. Our MLL generates [Formula: see text]4.8-ps optical pulses around 1065 nm at a repetition rate of ∼10 GHz, with energies exceeding 2.6 pJ and peak powers beyond 0.5 W. The repetition rate and the carrier-envelope offset frequency of the output can be controlled in a wide range by using the driving frequency and the pump current, providing a route for fully stabilized on-chip frequency combs.

Visible-to-mid-IR tunable frequency comb in nanophotonics.

Optical frequency comb is an enabling technology for a multitude of applications from metrology to ranging and communications. The tremendous progress in sources of optical frequency combs has mostly been centered around the near-infrared spectral region, while many applications demand sources in the visible and mid-infrared, which have so far been challenging to achieve, especially in nanophotonics. Here, we report widely tunable frequency comb generation using optical parametric oscillators in lithium niobate nanophotonics. We demonstrate sub-picosecond frequency combs tunable beyond an octave extending from 1.5 up to 3.3 µm with femtojoule-level thresholds on a single chip. We utilize the up-conversion of the infrared combs to generate visible frequency combs reaching 620 nm on the same chip. The ultra-broadband tunability and visible-to-mid-infrared spectral coverage of our source highlight a practical and universal path for the realization of efficient frequency comb sources in nanophotonics, overcoming their spectral sparsity.

Tunable and efficient ultraviolet generation with periodically poled lithium niobate.

On-chip ultraviolet (UV) sources are of great interest for building compact and scalable atomic clocks, quantum computers, and spectrometers. However, few material platforms are suitable for integrated UV light generation and manipulation. Of these materials, thin-film lithium niobate offers unique advantages such as sub-micron modal confinement, strong nonlinearity, and quasi-phase matching. Despite these characteristics, its utilization in the UV has remained elusive because of the substantial sensitivity of standard quasi-phase matching to fabrication imperfections, the photorefractive effect, and relatively large losses in this range. Here, we present efficient (197 ± 5%/W/cm2) second harmonic generation of UV-A light in a periodically poled lithium niobate nanophotonic waveguide. We achieve on-chip UV powers of ∼30 µW and linear wavelength tunability using temperature. These results are enabled with large cross section waveguides, which leads to first-order UV quasi-phase-matching with relatively long poling periods (>1.5 µm). By varying the poling period, we have achieved the shortest reported wavelength (355 nm) generated through frequency doubling in thin-film lithium niobate. Our results open up new avenues for UV on-chip sources and chip-scale photonics through compact frequency-doubling of common near-IR laser diodes.

Octave-spanning tunable infrared parametric oscillators in nanophotonics.

Widely tunable coherent sources are desirable in nanophotonics for a multitude of applications ranging from communications to sensing. The mid-infrared spectral region (wavelengths beyond 2 µm) is particularly important for applications relying on molecular spectroscopy. Among tunable sources, optical parametric oscillators typically offer some of the broadest tuning ranges; however, their implementations in nanophotonics have been limited to narrow tuning ranges in the infrared or to visible wavelengths. Here, we surpass these limits in dispersion-engineered periodically poled lithium niobate nanophotonics and demonstrate ultrawidely tunable optical parametric oscillators. Using 100 ns pulses near 1 µm, we generate output wavelengths tunable from 1.53 µm to 3.25 µm in a single chip with output powers as high as tens of milliwatts. Our results represent the first octave-spanning tunable source in nanophotonics extending into the mid-infrared, which can be useful for numerous integrated photonic applications.

Photonic elementary cellular automata for simulation of complex phenomena.

Cellular automata are a class of computational models based on simple rules and algorithms that can simulate a wide range of complex phenomena. However, when using conventional computers, these 'simple' rules are only encapsulated at the level of software. This can be taken one step further by simplifying the underlying physical hardware. Here, we propose and implement a simple photonic hardware platform for simulating complex phenomena based on cellular automata. Using this special-purpose computer, we experimentally demonstrate complex phenomena, including fractals, chaos, and solitons, which are typically associated with much more complex physical systems. The flexibility and programmability of our photonic computer present new opportunities to simulate and harness complexity for efficient, robust, and decentralized information processing using light.

Non-Abelian effects in dissipative photonic topological lattices.

Topology is central to phenomena that arise in a variety of fields, ranging from quantum field theory to quantum information science to condensed matter physics. Recently, the study of topology has been extended to open systems, leading to a plethora of intriguing effects such as topological lasing, exceptional surfaces, as well as non-Hermitian bulk-boundary correspondence. Here, we show that Bloch eigenstates associated with lattices with dissipatively coupled elements exhibit geometric properties that cannot be described via scalar Berry phases, in sharp contrast to conservative Hamiltonians with non-degenerate energy levels. This unusual behavior can be attributed to the significant population exchanges among the corresponding dissipation bands of such lattices. Using a one-dimensional example, we show both theoretically and experimentally that such population exchanges can manifest themselves via matrix-valued operators in the corresponding Bloch dynamics. In two-dimensional lattices, such matrix-valued operators can form non-commuting pairs and lead to non-Abelian dynamics, as confirmed by our numerical simulations. Our results point to new ways in which the combined effect of topology and engineered dissipation can lead to non-Abelian topological phenomena.

Mid-infrared cross-comb spectroscopy.

Dual-comb spectroscopy has been proven beneficial in molecular characterization but remains challenging in the mid-infrared region due to difficulties in sources and efficient photodetection. Here we introduce cross-comb spectroscopy, in which a mid-infrared comb is upconverted via sum-frequency generation with a near-infrared comb of a shifted repetition rate and then interfered with a spectral extension of the near-infrared comb. We measure CO2 absorption around 4.25 µm with a 1-µm photodetector, exhibiting a 233-cm-1 instantaneous bandwidth, 28000 comb lines, a single-shot signal-to-noise ratio of 167 and a figure of merit of 2.4 × 106 Hz1/2. We show that cross-comb spectroscopy can have superior signal-to-noise ratio, sensitivity, dynamic range, and detection efficiency compared to other dual-comb-based methods and mitigate the limits of the excitation background and detector saturation. This approach offers an adaptable and powerful spectroscopic method outside the well-developed near-IR region and opens new avenues to high-performance frequency-comb-based sensing with wavelength flexibility.

Few-cycle vacuum squeezing in nanophotonics.

One of the most fundamental quantum states of light is the squeezed vacuum, in which noise in one of the quadratures is less than the standard quantum noise limit. In nanophotonics, it remains challenging to generate, manipulate, and measure such a quantum state with the performance required for a wide range of scalable quantum information systems. Here, we report the development of a lithium niobate-based nanophotonic platform to demonstrate the generation and all-optical measurement of squeezed states on the same chip. The generated squeezed states span more than 25 terahertz of bandwidth supporting just a few optical cycles. The measured 4.9 decibels of squeezing surpass the requirements for a wide range of quantum information systems, demonstrating a practical path toward scalable ultrafast quantum nanophotonics.

The Fe3O4@apple seed starch core-shell structure decorated In(III): A green biocatalyst for the one-pot multicomponent synthesis of pyrazole-fused isocoumarins derivatives under solvent-free conditions.

In current decades, the fabrication and design of magnetic biocatalysts have been advancing as green catalysts. Hence, in this paper, we use the apple seed starch to create indium(III) immobilized on Fe3O4@apple seed starch core-shell magnetic nanocatalyst (Fe3O4@apple seed starch-In(III)). The prepared catalyst was identified and evaluated with several analysis techniques. The application of this catalyst in the synthesis of isochromeno[4,3-c]pyrazole-5(1H)-one derivates under solvent-free conditions was a new approach with high efficiency. Due to the magnetic nature of the catalyst, the catalyst separation from the reaction medium is easy, and it is reusable for five runs without significant change in catalytic activity. The fabrication of this catalyst is based on green chemistry principles and is more economical and stable than other catalysts in the synthesis of pyrazole-fused isocoumarins heterocyclic compounds.

Spectral phase transitions in optical parametric oscillators.

Driven nonlinear resonators provide a fertile ground for phenomena related to phase transitions far from equilibrium, which can open opportunities unattainable in their linear counterparts. Here, we show that optical parametric oscillators (OPOs) can undergo second-order phase transitions in the spectral domain between degenerate and non-degenerate regimes. This abrupt change in the spectral response follows a square-root dependence around the critical point, exhibiting high sensitivity to parameter variation akin to systems around an exceptional point. We experimentally demonstrate such a phase transition in a quadratic OPO. We show that the divergent susceptibility of the critical point is accompanied by spontaneous symmetry breaking and distinct phase noise properties in the two regimes, indicating the importance of a beyond nonlinear bifurcation interpretation. We also predict the occurrence of first-order spectral phase transitions in coupled OPOs. Our results on non-equilibrium spectral behaviors can be utilized for enhanced sensing, advanced computing, and quantum information processing.

Mie Resonance Engineering in Meta-Shell Supraparticles for Nanoscale Nonlinear Optics.

Supraparticles are coordinated assemblies of discrete nanoscale building blocks into complex and hierarchical colloidal superstructures. Holistic optical responses in such assemblies are not observed in an individual building block or in their bulk counterparts. Furthermore, subwavelength dimensions of the unit building blocks enable engraving optical metamaterials within the supraparticle, which thus far has been beyond the current pool of colloidal engineering. This can lead to effective optical features in a colloidal platform with ability to tune the electromagnetic responses of these particles. Here, we introduce and demonstrate the nanophotonics of meta-shell supraparticle (MSP), an all dielectric colloidal superstructure having an optical nonlinear metamaterial shell conformed onto a spherical core. We show that the metamaterial shell facilitates engineering the Mie resonances in the MSP that enable significant enhancement of the second harmonic generation (SHG). We show several orders of magnitude enhancement of second-harmonic generation in an MSP compared to its building blocks. Furthermore, we show an absolute conversion efficiency as high as 10-7 far from the damage threshold, setting a benchmark for SHG with low-index colloids. The MSP provides pragmatic solutions for instantaneous wavelength conversions with colloidal platforms that are suitable for chemical and biological applications. Their engineerability and scalability promise a fertile ground for nonlinear nanophotonics in the colloidal platforms with structural and material diversity.

Realizing spin Hamiltonians in nanoscale active photonic lattices.

Spin models arise in the microscopic description of magnetic materials and have been recently used to map certain classes of optimization problems involving large degrees of freedom. In this regard, various optical implementations of such Hamiltonians have been demonstrated to quickly converge to the global minimum in the energy landscape. Yet, so far, an integrated nanophotonic platform capable of emulating complex magnetic materials is still missing. Here, we show that the cooperative interplay among vectorial electromagnetic modes in coupled metallic nanolasers can be utilized to implement certain types of spin Hamiltonians. Depending on the topology/geometry of the arrays, these structures can be governed by a classical XY Hamiltonian that exhibits ferromagnetic and antiferromagnetic couplings, as well as geometrical frustration. Our results pave the way towards a scalable nanophotonic platform to study spin exchange interactions and could address a variety of optimization problems.

Multi-watt, broadband second-harmonic-generation in MgO:PPSLT waveguides fabricated with femtosecond laser micromachining.

We demonstrate optical waveguides fabricated in periodically poled MgO-doped stoichiometric lithium tantalate crystals using an fs-laser direct-write process. Two different waveguide architectures were developed: depressed cladding and stress-induced waveguides. Our strain-optic simulations confirmed the guiding mechanism for either case. We demonstrate designs optimized for low propagation loss (0.52 dB/cm) for both fundamental (1050 nm) and second-harmonic wavelengths (525 nm). Low-power CW second-harmonic-generation studies show normalized efficiencies comparable to that of annealed reverse-proton-exchange waveguides in lithium niobate. High-power studies demonstrate second-harmonic power levels up to 8.5 W in a single-pass configuration, using a 1-nm bandwidth CW IR fiber laser as a pump.

Experimental investigation of performance differences between coherent Ising machines and a quantum annealer.

Physical annealing systems provide heuristic approaches to solving combinatorial optimization problems. Here, we benchmark two types of annealing machines-a quantum annealer built by D-Wave Systems and measurement-feedback coherent Ising machines (CIMs) based on optical parametric oscillators-on two problem classes, the Sherrington-Kirkpatrick (SK) model and MAX-CUT. The D-Wave quantum annealer outperforms the CIMs on MAX-CUT on cubic graphs. On denser problems, however, we observe an exponential penalty for the quantum annealer [exp(-αDW N 2)] relative to CIMs [exp(-αCIM N)] for fixed anneal times, both on the SK model and on 50% edge density MAX-CUT. This leads to a several orders of magnitude time-to-solution difference for instances with over 50 vertices. An optimal-annealing time analysis is also consistent with a substantial projected performance difference. The difference in performance between the sparsely connected D-Wave machine and the fully-connected CIMs provides strong experimental support for efforts to increase the connectivity of quantum annealers.

Efficient half-harmonic generation of three-optical-cycle mid-IR frequency comb around 4 µm using OP-GaP.

We report a broadband mid-infrared frequency comb with three-optical-cycle pulse duration centered around 4.2 µm, via half-harmonic generation using orientation-patterned GaP (OP-GaP) with ~43% conversion efficiency. We experimentally compare performance of GaP with GaAs and lithium niobate as the nonlinear element, and show how properties of GaP at this wavelength lead to generation of the shortest pulses and the highest conversion efficiency. These results shed new light on half-harmonic generation of frequency combs, and pave the way for generation of short-pulse intrinsically-locked frequency combs at longer wavelengths in the mid-infrared with high conversion efficiencies.

Temporal Simultons in Optical Parametric Oscillators.

We report the first demonstration of a regime of operation in optical parametric oscillators (OPOs), in which the formation of temporal simultons produces stable femtosecond half-harmonic pulses. Simultons are simultaneous bright-dark solitons of a signal field at frequency ω and the pump field at 2ω, which form in a quadratic nonlinear medium. The formation of simultons in an OPO is due to the interplay of nonlinear pulse acceleration with the timing mismatch between the pump repetition period and the cold-cavity round-trip time and is evidenced by sech^{2} spectra with broad instantaneous bandwidths when the resonator is detuned to a slightly longer round-trip time than the pump repetition period. We provide a theoretical description of an OPO operating in a regime dominated by these dynamics, observe the distinct features of simulton formation in an experiment, and verify our results with numerical simulations. These results represent a new regime of operation in nonlinear resonators, which can lead to efficient and scalable sources of few-cycle frequency combs at arbitrary wavelengths.

A coherent Ising machine for 2000-node optimization problems.

The analysis and optimization of complex systems can be reduced to mathematical problems collectively known as combinatorial optimization. Many such problems can be mapped onto ground-state search problems of the Ising model, and various artificial spin systems are now emerging as promising approaches. However, physical Ising machines have suffered from limited numbers of spin-spin couplings because of implementations based on localized spins, resulting in severe scalability problems. We report a 2000-spin network with all-to-all spin-spin couplings. Using a measurement and feedback scheme, we coupled time-multiplexed degenerate optical parametric oscillators to implement maximum cut problems on arbitrary graph topologies with up to 2000 nodes. Our coherent Ising machine outperformed simulated annealing in terms of accuracy and computation time for a 2000-node complete graph.

A fully programmable 100-spin coherent Ising machine with all-to-all connections.

Unconventional, special-purpose machines may aid in accelerating the solution of some of the hardest problems in computing, such as large-scale combinatorial optimizations, by exploiting different operating mechanisms than those of standard digital computers. We present a scalable optical processor with electronic feedback that can be realized at large scale with room-temperature technology. Our prototype machine is able to find exact solutions of, or sample good approximate solutions to, a variety of hard instances of Ising problems with up to 100 spins and 10,000 spin-spin connections.

A 16-bit Coherent Ising Machine for One-Dimensional Ring and Cubic Graph Problems.

Many tasks in our modern life, such as planning an efficient travel, image processing and optimizing integrated circuit design, are modeled as complex combinatorial optimization problems with binary variables. Such problems can be mapped to finding a ground state of the Ising Hamiltonian, thus various physical systems have been studied to emulate and solve this Ising problem. Recently, networks of mutually injected optical oscillators, called coherent Ising machines, have been developed as promising solvers for the problem, benefiting from programmability, scalability and room temperature operation. Here, we report a 16-bit coherent Ising machine based on a network of time-division-multiplexed femtosecond degenerate optical parametric oscillators. The system experimentally gives more than 99.6% of success rates for one-dimensional Ising ring and nondeterministic polynomial-time (NP) hard instances. The experimental and numerical results indicate that gradual pumping of the network combined with multiple spectral and temporal modes of the femtosecond pulses can improve the computational performance of the Ising machine, offering a new path for tackling larger and more complex instances.