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Miniaturizing nonlinear optical components is essential for integrating advanced light manipulation into compact photonic devices, enabling scalable and cost-effective applications. While monocrystalline lithium niobate thin films advance nonlinear nanophotonics, their high inertness limits the design of top-down fabricated nanostructures. Here we present a versatile bottom-up fabrication method based on nanoimprint lithography for achieving polycrystalline lithium niobate nanostructures, and demonstrate its significant potential for nonlinear metasurfaces. The fabrication enables nearly vertical features and aspect ratios of up to 6, which we combine with a novel solution-derived material with high effective second-order nonlinearity of d_{eff}=5 pm/V. On this platform, we demonstrate second-harmonic focusing over a broad spectral range from near-UV to near-IR, increasing the nonlinear signal intensity by up to 34 times. Our method enables the first lithium niobate metalens and expands the field of nonlinear metasurfaces by providing a low-cost, highly scalable fabrication method for engineered nonlinear nanostructures

Nonlinear disordered media uniquely combine multiple scattering and second-harmonic generation. Here, we investigate the statistical properties of the nonlinear light generated within such media. We report super-Rayleigh statistics of the second-harmonic speckle intensity, and demonstrate that it is caused by the mesoscopic correlations arising in extreme scattering conditions. The measured conductance is the lowest ever observed in an isotropically scattering 3D medium, with applications in broadband second-harmonic generation, wavefront shaping in nonlinear disordered media, and photonic computing., Comment: 13 pages, 10 figures

Optical quantum communication technologies are making the prospect of unconditionally secure and efficient information transfer a reality. The possibility of generating and reliably detecting quantum states of light, with the further need of increasing the private data-rate is where most research efforts are focusing. The physical concept of entanglement is a solution guaranteeing the highest degree of security in device-independent schemes, yet its implementation and preservation over long communication links is hard to achieve. Lithium niobate-on-insulator has emerged as a revolutionising platform for high-speed classical telecommunication and is equally suited for quantum information applications owing to the large second-order nonlinearities that can efficiently produce entangled photon pairs. In this work, we generate maximally entangled quantum states in the time-bin basis using lithium niobate-on-insulator photonics at the fibre optics telecommunication wavelength, and reconstruct the density matrix by quantum tomography on a single photonic integrated circuit. We use on-chip periodically-poled lithium niobate as source of entangled qubits with a brightness of 242 MHz/mW and perform quantum tomography with a fidelity of 91.9+-1.0 %. Our results, combined with the established large electro-optic bandwidth of lithium niobate, showcase the platform as perfect candidate to realise fibre-coupled, high-speed time-bin quantum communication modules that exploit entanglement to achieve information security.

Polarization-entangled photon pair sources are essential for diverse quantum technologies, such as quantum communication, computation, and imaging. However, the generation of complex polarization-entangled quantum states has long been constrained by the available nonlinear susceptibility tensor of natural nonlinear crystals, necessitating a cumbersome and intricate setup for additional coherent superposition or post-selection. In this study, we introduce and experimentally demonstrate a nanoscale polarization-entangled photon pair source utilizing an artificially-engineered metamaterial platform. This platform is based on a plasmonic metasurface that is strongly coupled to an epsilon-near-zero (ENZ) material. By precisely engineering resonances at both pump and signal/idler wavelengths, and leveraging the field enhancement provided by the ENZ effect, the photon pair generation efficiency of the 68-nm-thick metasurface is significantly boosted. More notably, the ENZ metasurface platform facilitates versatile manipulation of the system's anisotropic second-order nonlinear susceptibility tensor, enabling direct control over the polarization states of the photon pairs, which leads to the generation of a polarization-entangled Bell state without the need for additional components. Our approach opens a new avenue for the simultaneous photon pair generation and quantum state engineering in a compact platform.

Intensity modulators are fundamental components for integrated photonics. From near infrared to visible spectral ranges, they find applications in optical communication and quantum technologies. In particular, they are required for the control and manipulation of atomic systems such as atomic clocks and quantum computers. Typical integrated electro-optic modulators operating at these wavelengths show high bandwidth and low voltage operation, but their extinction ratios are moderate. Here we present an integrated thin-film lithium niobate electro-optic modulator operating in the C-band, which uses a subsequent periodically poled waveguide to convert the modulated signal from 1536 nm to 768 nm using second harmonic generation. We demonstrate that the upconverted signal retains the characteristics of the modulated input signal, reaching a measured high bandwidth of 40 GHz. Due to the nature of the nonlinear process, it exhibits, with respect to the fundamental signal, a doubled extinction ratio of 46 dB, which is the highest recorded for near-infrared light on this platform., Comment: 4 pages, 3 figures

Generating and interfering non-classical states of light is fundamental to optical quantum information science and technology. Quantum photonic integrated circuits provide one pathway towards scalability by combining nonlinear sources of non-classical light and programmable circuits in centimeter-scale devices. The key requirements for quantum applications include efficient generation of indistinguishable photon-pairs and high-visibility programmable quantum interference. Here, we demonstrate a lithium niobate-on-insulator (LNOI) integrated photonic circuit that generates a two-photon path-entangled state, and a programmable interferometer for quantum interference. We generate entangled photons with $\sim2.3\times10^8$ pairs/s/mW brightness and perform quantum interference experiments on the chip with $96.8\pm3.6\%$ visibility. LNOI is an emerging photonics technology that has revolutionized high-speed modulators and efficient frequency conversion. Our results provide a path towards large-scale integrated quantum photonics including efficient photon-pair generation and programmable circuits for applications such as boson sampling and quantum communications.

Second harmonic generation (SHG) is prohibited in centrosymmetric crystals such as silicon or germanium due to the presence of inversion symmetry. However, the structuring of such materials makes it possible to break the inversion symmetry, thus achieving generation of second-harmonic. Moreover, various symmetry properties of the resulting structure, such as chirality, also influence the SHG. In this work we investigate second harmonic generation from an array of nanohelices made of germanium. The intensity of the second harmonic displayed a remarkable enhancement of over 100 times compared to a non-structured Ge thin film, revealing the influence of interaction between nanohelices. In particular, nonlinear circular dichroism, characterized through the SHG anisotropy factor g, changed its sign not only with the helix handedness, but with its density as well. We believe that our discoveries will open up new paths for the development of nonlinear photonics based on metamaterials and metasurfaces made of centrosymmetric materials., Comment: 16 pages, 5 figures

Neural networks find widespread use in scientific and technological applications, yet their implementations in conventional computers have encountered bottlenecks due to ever-expanding computational needs. Photonic neuromorphic hardware, which manipulates information and represents data continuously in the optical domain, is one of the promising platforms with potential advantages of massive parallelism, ultralow latency, and reduced energy consumption. While linear photonic neural networks are within reach, photonic computing with large-scale optical nonlinear nodes remains largely unexplored. Here, we demonstrate a large-scale, high-performance nonlinear photonic neural system based on a disordered polycrystalline slab composed of lithium niobate nanocrystals. Mediated by random quasi-phase-matching and multiple scattering, linear and nonlinear optical speckle features are generated as the interplay between the simultaneous linear random scattering and the second-harmonic generation, defining a complex neural network in which the second-order nonlinearity acts as internal nonlinear activation functions. Benchmarked against linear random projection, such nonlinear mapping embedded with rich physical computational operations shows improved performance across a large collection of machine learning tasks in image classification, regression, and graph classification with varying complexity. Demonstrating up to 27,648 input and 3,500 nonlinear output nodes, the combination of optical nonlinearity and random scattering serves as a scalable computing engine for diverse applications.

Nonlinear optical effects are used to generate coherent light at wavelengths difficult to reach with lasers. Materials periodically poled or nanostructured in the nonlinear susceptibility in three spatial directions are called 3D nonlinear photonic crystals (NPhCs). They enable enhanced nonlinear optical conversion efficiencies, emission control, and simultaneous generation of nonlinear wavelengths. The chemical inertness of efficient second-order nonlinear materials ($\chi^{(2)}$) prohibited their nanofabrication until 2018. The current method is restricted to top-down laser-based techniques limiting the periodicity along z-axis to 10 um. We demonstrate the first bottom-up fabricated 3D NPhC in sol-gel derived barium titanate by soft-nanoimprint lithography: a woodpile with eight layers and periodicities of 1 um (xy-plane) and 300 nm (z-plane). The surface areas exceed $5.3\cdot 10^4$ um^2, which is two orders of magnitude larger than the state-of-the-art. This study is expected to initiate bottom-up fabrication of 3D NPhCs with a supremely strong and versatile nonlinear response., Comment: 11 pages, 4 figures

The quest of a nonlinear optical material that can be easily nanostructured over a large surface area is still ongoing. Here, we demonstrate a nanoimprinted nonlinear barium titanate 2D nanohole array that shows optical properties of a 2D photonic crystal and metasurface, depending on the direction of the optical axis. The challenge of nanostructuring the inert metal-oxide is resolved by direct soft nanoimprint lithography with sol-gel derived barium titanate enabling critical dimensions of 120 nm with aspect ratios of 5. The nanohole array exhibits a photonic bandgap in the infrared range when probed along the slab axis while lattice resonant states are observed in out-of-plane transmission configuration. The enhanced light-matter interaction from the resonant structure enables to increase the second-harmonic generation in the near-UV by a factor of 18 illustrating the potential in the flexible fabrication technique for barium titanate photonic devices.

We present a graph-based model for multiple scattering of light in integrated lithium niobate on insulator (LNOI) networks, which describes an open network of single-mode integrated waveguides with tunable scattering at the network nodes. We first validate the model at small scale with experimental LNOI resonator devices and show consistent agreement between simulated and measured spectral data. Then, the model is used to demonstrate a novel platform for on-chip multiple scattering in large-scale optical networks up to few hundred nodes, with tunable scattering behaviour and tailored disorder. Combining our simple graph-based model with material properties of LNOI, this platform creates new opportunities to control randomness in large optical networks.

Quantum computers comprise elementary logic gates that initialize, control and measure delicate quantum states. One of the most important gates is the controlled-NOT, which is widely used to prepare two-qubit entangled states. The controlled-NOT gate for single photon qubits is normally realized as a six-mode network of individual beamsplitters. This architecture however, utilizes only a small fraction of the circuit for the quantum operation with the majority of the footprint dedicated to routing waveguides. Quantum walks are an alternative photonics platform that use arrays of coupled waveguides with a continuous interaction region instead of discrete gates. While quantum walks have been successful for investigating condensed matter physics, applying the multi-mode interference for logical quantum operations is yet to be shown. Here, we experimentally demonstrate a two-qubit controlled-NOT gate in an array of lithium niobate-on-insulator waveguides. We engineer the tight-binding Hamiltonian of the six evanescently-coupled single-mode waveguides such that the multi-mode interference corresponds to the linear optical controlled-NOT unitary. We measure the two-qubit transfer matrix with $0.938\pm0.003$ fidelity, and we use the gate to generate entangled qubits with $0.945\pm0.002$ fidelity by preparing the control photon in a superposition state. Our results highlight a new application for quantum walks that use a compact multi-mode interaction region to realize large multi-component quantum circuits.

Quantum emitters in solid-state crystals have recently attracted a lot of attention due to their simple applicability in optical quantum technologies. The polarization of single photons generated by quantum emitters is one of the key parameters that play a crucial role in the applications, such as quantum computation that uses the indistinguishability of photons. However, the degree of single photon polarization is typically quantified using time-averaged photoluminescence intensity of single emitters, which provides limited information about the dipole properties in solids. In this work, we use single defects in hexagonal boron nitride and nanodiamond as efficient room-temperature single photon sources to reveal the origin and the temporal evolution of dipole orientation in solid-state quantum emitters. The angle of excitation and emission dipoles relative to the crystal axes are determined experimentally and then calculated using density functional theory, which results in characteristic angles for every specific defect that can be used as an efficient tool for defect identification and understanding their atomic structure. Moreover, the temporal polarization dynamics reveal a strongly modified linear polarization visibility that depends on the excited state decay time of individual excitation. This effect can be traced back potentially to the excitation of excess charges in the local crystal environment. Understanding such hidden time-dependent mechanisms can further be used to improve the performance of polarization-sensitive experiments, in particular that of quantum communication with single photon emitters.

Modern machine learning models use an ever-increasing number of parameters to train (175 billion parameters for GPT-3) with large datasets to obtain better performance. Bigger is better has been the norm. Optical computing has been reawakened as a potential solution to large-scale computing through optical accelerators that carry out linear operations while reducing electrical power. However, to achieve efficient computing with light, creating and controlling nonlinearity optically rather than electronically remains a challenge. This study explores a reservoir computing (RC) approach whereby a 14 mm long few-mode waveguide in LiNbO3 on insulator is used as a complex nonlinear optical processor. A dataset is encoded digitally on the spectrum of a femtosecond pulse which is then launched in the waveguide. The output spectrum depends nonlinearly on the input. We experimentally show that a simple digital linear classifier with 784 parameters using the output spectrum from the waveguide as input increased the classification accuracy of several databases compared to non-transformed data, approximately 10$\%$. In comparison, a deep digital neural network (NN) with 40000 parameters was necessary to achieve the same accuracy. Reducing the number of parameters by a factor of $\sim$50 illustrates that a compact optical RC approach can perform on par with a deep digital NN., Comment: 13 pages, 3 figures and 1 table

We present a wearable device with III-V nanowires in a flexible polymer, which is used for active mechanical tuning of the second-harmonic generation intensity. An array of vertical GaAs nanowires was grown with metalorganic vapour-phase epitaxy, then embedded in polydimethylsiloxane and detached from the rigid substrate with mechanical peel off. Experimental results show a tunability of the second-harmonic generation intensity by a factor of two for 30% stretching which matches the simulations including the distribution of sizes. We studied the impact of different parameters on the band dispersion and tunability of the second-harmonic generation, such as the pitch, the length, and the diameter. We predict at least three orders of magnitude active mechanical tuning of the nonlinear signal intensity for nanowire arrays. The flexibility of the array together with the resonant wavelength engineering make such structures perspective platforms for future bendable or stretchable nanophotonic devices as light sources or sensors., Comment: Paper has 18 pages and 5 figures

Nonclassical light sources are highly sought after as they are an integral part of quantum communication and quantum computation devices. Typical sources rely on bulk crystals that are not compact and have limited bandwidth due to phase-matching conditions. In this work, we demonstrate the generation of photon pairs from a free-standing lithium niobate microcube at the telecommunication wavelength through the spontaneous parametric down-conversion process. The maximum photon pair generation rate obtained from a single microcube with the size of ~4 microns is ~80 Hz, resulting in an efficiency of ~1.2 GHz/Wm per unit volume, which is an order of magnitude higher than the efficiency of photon-pair generation in bulky nonlinear crystals. The microcubes are synthesized through a solvothermal method, offering the possibility for scalable devices via bottom-up assembly. Our work constitutes an important step forward in the realization of compact nonclassical light sources with broadband tunability for various applications in quantum communication, quantum computing, and quantum metrology., Comment: 19 pages, 4 figures

In display technologies or data processing, planar and subwavelength free-space components suited for flat photonic devices are needed. Metasurfaces, which shape the optical wavefront within hundreds of nanometers, can provide a solution for thin and portable photonic devices, e.g. as CMOS-compatible modules. While conventional electro-optic modulators are inconvenient to operate in free space configurations, its principle can largely be applied to the development of active metasurfaces with the prospect of modulation speeds up to the GHz region. Here, we use this concept to realize fast and continuous modulation of light at low voltage and MHz speed with a lithium niobate metasurface tuned by the linear electro-optic effect. Furthermore, we exploit the resonance in the visible to enhance the modulation of the transmitted light by two orders of magnitude, namely by a factor of 80, compared to the unstructured substrate. This proof-of-concept work is a first important step towards the use of lithium niobate metasurfaces for free space modulation.

We provide a vectorial model to simulate second-harmonic generation (SHG) in birefringent, transparent media with an arbitrary configuration of non-linear ($\chi^{(2)}$) crystalline grains. We apply this model on disordered assemblies of LiNbO$_3$ and BaTiO$_3$ grains to identify the influence of the birefringence on the random quasi-phase-matching process. We show that in monodispersed assemblies, the birefringence relaxes the grain-size dependence of the SHG efficiency. In polydispersed assemblies with sufficiently large grains, we find that the birefringence introduces an SHG efficiency enhancement of up to 54% compared to isotropic reference crystals, which is grain size independent. This enhancement increases linearly with the grain size, if the birefringent grains can be phase matched. These two different scaling behaviours are used in Kurtz and Perry's powder-technique to identify the phase-matchability of a material. We show on the example of LiNbO$_3$ and ADP that this technique cannot be applied when the grains get smaller than the coherence length, because the SHG scaling with the grain size becomes material specific., Comment: Main: 7 pages, 4 Figures. Supplementaries: 11 pages, 8 figures

High-quality crystals without inversion symmetry are the conventional platform to achieve optical frequency conversion via three wave-mixing. In bulk crystals, efficient wave-mixing relies on phase-matching configurations, while at the micro- and nano-scale it requires resonant mechanisms that enhance the nonlinear light-matter interaction. These strategies commonly result in wavelength-specific performances and narrowband applications. Disordered photonic materials, made up of a random assembly of optical nonlinear crystals, enable a broadband tunability in the random quasi-phase-matching (RQPM) regime and do not require high-quality materials. Here, we combine resonances and disorder by implementing RQPM in Mie-resonant spheres of a few microns realized by the bottom-up assembly of barium titanate nano-crystals. The measured second harmonic generation (SHG) reveals a combination of broadband and resonant wave mixing, in which Mie resonances drive and enhance the SHG, while the disorder keeps the phase-matching conditions relaxed. This new phase-matching regime can be described by a random walk in the SHG complex plane whose step lengths depend on the local field enhancement within the micro-sphere. Our nano-crystals assemblies provide new opportunities for tailored phase-matching at the micro-scale, beyond the coherence length of the bulk crystal. They can be adapted to achieve frequency conversion from the near-ultraviolet to the infrared ranges, they are low-cost and scalable to large surface areas., Comment: Main: 9 pages, 5 Figures. Supplementaries: 24 pages, 11 figures, 1 table

On January 13th 2020, the inaugural Photonics Online Meetup (POM) brought together more than 1100 researchers to discuss the latest advances in photonics. Or rather, it didn't, because the meeting was completely delocalized with the speakers, organizers, and attendees scattered across six continents and hundreds of locations, connected via a video-conferencing tool and social media. Despite this "delocalisation," the meeting retained many characteristics of a traditional conference: invited and contributed talks with follow-up questions and discussion, and a poster session. However, unlike with traditional conferences, all attendees avoided air travel, high registration costs (it was completely free), CO2 emission, or visa issues. Surely the impact on families was minimized as well, though participants in inconvenient time zones had to wake up early or stay up late. In this Comment, we highlight the key steps that enabled this event, offering tips and advice, to aid the organisation of similar Online Meetups., Comment: Updated some of the text and added a figure

Nonradiating electromagnetic configurations in nanostructures open new horizons for applications due to two essential features: lack of energy losses and invisibility to the propagating electromagnetic field. Such radiationless configurations form a basis for new types of nanophotonic devices, where a strong electromagnetic field confinement can be achieved together with lossless interactions between nearby components. In our work, we present a new design of free-standing disk nanoantennas with nonradiating current distributions for the optical near-infrared range. We show a novel approach to create nanoantennas by slicing III-V nanowires into standing disks using focused ion beam milling. We experimentally demonstrate the suppression of the far-field radiation and the associated strong enhancement of the second-harmonic generation from the disk nanoantennas. With a theoretical analysis of the electromagnetic field distribution using multipole expansions in both spherical and Cartesian coordinates, we confirm that the demonstrated nonradiating configurations are anapoles. We expect that the presented procedure to design and produce disk nanoantennas from nanowires become one of standard approaches to fabricate controlled chains of standing nanodisks with different designs and configurations. These chains can be an essential building blocks for new types of lasers and sensors with low power consumption.