Nanoimprinting Solution-Derived Barium Titanate for Electro-Optic Metasurfaces.

Electro-optic metasurfaces have demonstrated significant potential in enhancing the modulation speed and efficiency for fast and large-scale free-space optical devices. Barium titanate has a strong electro-optic Pockels coefficient, but its availability in thin-film form is restricted due to costly growth processes or low thickness. Here, we fabricated active metasurfaces using an etch-free bottom-up process with sol-gel-based polycrystalline barium titanate with a large electro-optic coefficient similar to bulk lithium niobate. We achieve strong hybrid Mie/surface lattice resonances with a quality-factor of 200 at 633 nm wavelength, enhancing the light-matter interaction and therefore the Pockels effect. The metasurface transmission is electro-optically modulated with up to 5 MHz driving frequency at low voltages of less than 1 V thanks to resonant enhancement of the modulation amplitude by 2 orders of magnitude. This successful demonstration of electro-optic modulation in nanoimprinted barium titanate structures paves the way for low-cost and large-scale free-space modulators or tunable metalenses.

Background-Free Near-Infrared Biphoton Emission from Single GaAs Nanowires.

The generation of photon pairs from nanoscale structures with high rates is still a challenge for the integration of quantum devices, as it suffers from parasitic signals from the substrate. In this work, we report type-0 spontaneous parametric down-conversion at 1550 nm from individual bottom-up grown zinc-blende GaAs nanowires with lengths of up to 5 µm and diameters of up to 450 nm. The nanowires were deposited on a transparent ITO substrate, and we measured a background-free coincidence rate of 0.05 Hz in a Hanbury-Brown-Twiss setup. Taking into account transmission losses, the pump fluence, and the nanowire volume, we achieved a biphoton generation of 60 GHz/Wm, which is at least 3 times higher than that of previously reported single nonlinear micro- and nanostructures. We also studied the correlations between the second-harmonic generation and the spontaneous parametric down-conversion intensities with respect to the pump polarization and in different individual nanowires.

Sol-Gel Barium Titanate Nanohole Array as a Nonlinear Metasurface and a Photonic Crystal.

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 the optical properties of a 2D photonic crystal and a 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 five. 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 in the second-harmonic generation in the near-ultraviolet by a factor of 18 illustrating the potential in the flexible fabrication technique for barium titanate photonic devices.

Graph model for multiple scattering in lithium niobate on insulator integrated photonic networks.

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.

High-bandwidth thermo-optic phase shifters for lithium niobate-on-insulator photonic integrated circuits.

Phase shifters are key components of large-scale photonic integrated circuits. For the lithium niobate-on-insulator (LNOI) platform, thermo-optic phase shifters (TOPS) have emerged as a more stable and compact alternative to common electro-optic phase shifters (EOPSs), which are prone to anomalous behavior and drifting at low frequencies. Here, we model and experimentally characterize the influence of geometry on the performance of metal strip TOPSs. Compared to EOPSs, a 10-fold reduction of the voltage-length product is measured and bandwidths beyond 100 kHz are demonstrated, while keeping the footprint as low as 0.04 mm2. This shows the potential of TOPSs as small-scale building blocks for stable tuning and switching in LNOI photonic circuits.

Mapping of Fabry-Perot and whispering gallery modes in GaN microwires by nonlinear imaging.

Engineering nonlinear optical responses at the microscale is a key topic in photonics for achieving efficient frequency conversion and light manipulation. Gallium nitride (GaN) is a promising semiconductor material for integrated nonlinear photonic structures. In this work, we use epitaxially grown GaN microwires as nonlinear optical whispering gallery and Fabry-Perot resonators. We demonstrate an effective generation of second-harmonic and polarization-dependent signals of whispering gallery and Fabry-Perot modes (FPM) under near-infrared (NIR) excitation. We show how the rotation of the excitation polarization can be used to control and switch between Fabry-Perot and whispering gallery modes in tapered GaN microwire resonators. We demonstrate the enhancement of two-photon luminescence in the yellow-green spectral range due to efficient coupling between whispering gallery, FPM, and excitonic states in GaN. This luminescence enhancement allows us to conveniently visualize whispering gallery modes excited with a NIR source. Such microwire resonators can be used as compact microlasers or sensing elements in photonic sensors.

Reshaping the Second-Order Polar Response of Hybrid Metal-Dielectric Nanodimers.

We combine the field confinement of plasmonics with the flexibility of multiple Mie resonances by bottom-up assembly of hybrid metal-dielectric nanodimers. We investigate the electromagnetic coupling between nanoparticles in heterodimers consisting of gold and barium titanate (BaTiO3 or BTO) nanoparticles through nonlinear second-harmonic spectroscopy and polarimetry. The overlap of the localized surface plasmon resonant dipole mode of the gold nanoparticle with the dipole and higher-order Mie resonant modes in the BTO nanoparticle lead to the formation of hybridized modes in the visible spectral range. We employ the pick-and-place technique to construct the hybrid nanodimers with controlled diameters by positioning the nanoparticles of different types next to each other under a scanning electron microscope. Through linear scattering spectroscopy, we observe the formation of hybrid modes in the nanodimers. We show that the modes can be directly accessed by measuring the dependence of the second-harmonic generation (SHG) signal on the polarization and wavelength of the pump. We reveal both experimentally and theoretically that the hybridization of plasmonic and Mie-resonant modes leads to a strong reshaping of the SHG polarization dependence in the nanodimers, which depends on the pump wavelength. We compare the SHG signal of each hybrid nanodimer with the SHG signal of single BTO nanoparticles to estimate the enhancement factor due to the resonant mode coupling within the nanodimers. We report up to 2 orders of magnitude for the SHG signal enhancement compared with isolated BTO nanoparticles.

Image-based autofocusing system for nonlinear optical microscopy with broad spectral tuning.

We present an image-based autofocusing system applied in nonlinear microscopy and spectroscopy with a wide range of excitation wavelengths. The core of the developed autofocusing system consists of an adapted two-step procedure maximizing an image score with six different image scorings algorithms implemented to cover different types of focusing scenarios in automated regime for broad wavelength region. The developed approach is combined with an automated multi-axis alignment procedure. We demonstrate the key abilities of the autofocusing procedure on different types of structures: single nanoparticles, nanowires and complex 3D nanostructures. Based on these experiments, we determine the optimal autofocusing algorithms for different types of structures and applications.

Anapoles in Free-Standing III-V Nanodisks Enhancing Second-Harmonic Generation.

Nonradiating electromagnetic configurations in nanostructures open new horizons for applications due to two essential features: a lack of energy losses and invisibility to the propagating electromagnetic field. Such radiationless configurations form a basis for new types of nanophotonic devices, in which 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 creating 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 of designing and producing disk nanoantennas from nanowires becomes one of the standard approaches to fabricating controlled chains of standing nanodisks with different designs and configurations. These chains can be essential building blocks for new types of lasers and sensors with low power consumption.

Extreme electro-optic tuning of Bragg mirrors integrated in lithium niobate nanowaveguides.

Bragg reflectors (BRFs) are essential elements in optical telecommunication and sensing applications. Their miniaturization down to the sub-micron scale has been achieved in silicon-on-insulator chips. However, their tunability is limited only to thermal tuning. In order to achieve a faster and more practical tunability operation, here we report on electro-optically tunable BRFs with ∼14 dB signal filtering on a lithium-niobate-on-insulator platform, while keeping sub-micron cross-sections. Due to the lithium niobate electro-optic properties and the chosen electrodes configuration, a Bragg tunability coefficient of 23.37±0.55 pm/V is achieved, which enhances ∼33 times the tunability performance of state-of-the-art BRFs.

Enhanced Second-Harmonic Generation from Sequential Capillarity-Assisted Particle Assembly of Hybrid Nanodimers.

We show enhanced second-harmonic generation (SHG) from a hybrid metal-dielectric nanodimer consisting of an inorganic perovskite nanoparticle of barium titanate (BaTiO3) coupled to a metallic gold (Au) nanoparticle. BaTiO3-Au nanodimers of 100 nm/80 nm sizes are fabricated by sequential capillarity-assisted particle assembly. The BaTiO3 nanoparticle has a noncentrosymmetric crystalline structure and generates bulk SHG. We use the localized surface plasmon resonance of the gold nanoparticle to enhance the SHG from the BaTiO3 nanoparticle. We experimentally measure the nonlinear signal from assembled nanodimers and demonstrate an up to 15-fold enhancement compared to a single BaTiO3 nanoparticle. We further perform numerical simulations of the linear and SHG spectra of the BaTiO3-Au nanodimer and show that the gold nanoparticle acts as a nanoantenna at the SHG wavelength.

Nonlinear mode switching in lithium niobate nanowaveguides to control light directionality.

The ability of nanowaveguides to confine and guide light has been applied for developing optical applications such as nanolasers, optical switching and localized imaging. These and others applications can be further complemented by the optical control of the guided modes within the nanowaveguide, which in turn dictates the light emission pattern. It has been shown that the light directionality can be shaped by varying the nanowire cross-sections. Here, we demonstrate that the directionality of the light can be modified using a single nanowaveguide with a nonlinear phenomenon such as second-harmonic generation. In individual lithium niobate nanowaveguides, we use second-harmonic modal phase-matching and we apply it to switch the guided modes within its sub-micron cross-section. In doing so, we can vary the light directionality of the generated light from straight (0° with respect to the propagation direction) to large spread angles (almost 54°). Further, we characterize the directionality of the guided light by means of optical Fourier transformation and show that the directionality of the guided light changes for different wavelengths.

Polar Second-Harmonic Imaging to Resolve Pure and Mixed Crystal Phases along GaAs Nanowires.

In this work, we report an optical method for characterizing crystal phases along single-semiconductor III-V nanowires based on the measurement of polarization-dependent second-harmonic generation. This powerful imaging method is based on a per-pixel analysis of the second-harmonic-generated signal on the incoming excitation polarization. The dependence of the second-harmonic generation responses on the nonlinear second-order susceptibility tensor allows the distinguishing of areas of pure wurtzite, zinc blende, and mixed and rotational twins crystal structures in individual nanowires. With a far-field nonlinear optical microscope, we recorded the second-harmonic generation in GaAs nanowires and precisely determined their various crystal structures by analyzing the polar response for each pixel of the images. The predicted crystal phases in GaAs nanowire are confirmed with scanning transmission electron and high-resolution transmission electron measurements. The developed method of analyzing the nonlinear polar response of each pixel can be used for an investigation of nanowire crystal structure that is quick, sensitive to structural transitions, nondestructive, and on-the-spot. It can be applied for the crystal phase characterization of nanowires built into optoelectronic devices in which electron microscopy cannot be performed (for example, in lab-on-a-chip devices). Moreover, this method is not limited to GaAs nanowires but can be used for other nonlinear optical nanostructures.

Fabrication of free-standing lithium niobate nanowaveguides down to 50 nm in width.

Nonlinear optical nanoscale waveguides are a compact and powerful platform for efficient wavelength conversion. The free-standing waveguide geometry opens a range of applications in microscopy for local delivery of light, where in situ wavelength conversion helps to overcome various wavelength-dependent issues, such as biological tissue damage. In this paper, we present an original patterning method for high-precision fabrication of free-standing nanoscale waveguides based on lithium niobate, a material with a strong second-order nonlinearity and a broad transparency window covering the visible and mid-infrared wavelength ranges. The fabrication process combines electron-beam lithography with ion-beam enhanced etching and produces nanowaveguides with lengths from 5 to 50 µm, widths from 50 to 1000 nm and heights from 50 to 500 nm, each with a precision of few nanometers. The fabricated nanowaveguides are tested in an optical characterization experiment showing efficient second-harmonic generation.

Fabrication of nanoscale lithium niobate waveguides for second-harmonic generation.

Nanoscale waveguides are basic building blocks of integrated optical devices. Especially, waveguides made from nonlinear optical materials, such as lithium niobate, allow access to a broad range of applications using second-order nonlinear frequency conversion processes. Based on a lithium niobate on insulator substrate, millimeter-long nanoscale waveguides were fabricated with widths as small as 200 nm. The fabrication was done by means of potassium hydroxide-assisted ion-beam-enhanced etching. The waveguides were optically characterized in the near infrared wavelength range showing phase-matched second-harmonic generation.

Monolithic thin-film lithium niobate broadband spectrometer with one nanometre resolution.

Miniaturised optical spectrometers are attractive due to their small footprint, low weight, robustness and stability even in harsh environments such as space or industrial facilities. We report on a stationary-wave integrated Fourier-transform spectrometer featuring a measured optical bandwidth of 325 nm and a theoretical spectral resolution of 1.2 nm. We fabricate and test on lithium niobate-on-insulator to take full advantage of the platform, namely electro-optic modulation, broad transparency range and the low optical loss achieved thanks to matured fabrication techniques. We use the electro-optic effect and develop innovative layouts to overcome the undersampling limitations and improve the spectral resolution, thus providing a framework to enhance the performance of all devices sharing the same working principle. With our work, we add another important element to the portfolio of integrated lithium-niobate optical devices as our spectrometer can be combined with multiple other building blocks to realise functional, monolithic and compact photonic integrated circuits.

Large-scale photonic computing with nonlinear disordered media.

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 computing is a promising neuromorphic platform with potential advantages of massive parallelism, ultralow latency and reduced energy consumption but mostly for computing linear operations. 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. 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.

Polarization Dynamics of Solid-State Quantum Emitters.

Quantum emitters in solid-state crystals have recently attracted a great deal 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 plays a crucial role in various applications, such as quantum computation, which uses the indistinguishability of photons. However, the degree of single-photon polarization is typically quantified using the 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 temporal evolution of the dipole orientation in solid-state quantum emitters. The angles of the excitation and emission dipoles relative to the crystal axes were determined experimentally and then calculated using density functional theory, which resulted 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 revealed a strongly modified linear polarization visibility that depends on the excited-state decay time of the individual excitation. This effect can potentially be traced back to the excitation of excess charges in the local crystal environment. Understanding such hidden time-dependent mechanisms can further improve the performance of polarization-sensitive experiments, particularly that for quantum communication with single-photon emitters.

Second-harmonic generation in lithium niobate nanowires for local fluorescence excitation.

We study the nonlinear optical properties of lithium niobate (LiNbO(3)) nanowires (NWs) fabricated by a top-down ion beam enhanced etching method. First, we demonstrate generation and propagation of the second-harmonic (SH) light in LiNbO(3) NWs of typical rectangular cross-sections of 400 x 600 nm(2) and length from 10 to 50 µm. Then, we show local fluorescent excitation of 4',6-diamidino-2-phenylindole (DAPI) dye with the propagated SH signal in standard concentrations as for biological applications. By measuring the detected average power of the propagated fundamental harmonic (FH) and the SH signal at the output of the NWs, we directly prove the dominating role of the SH signal over possible two-photon excitation processes with the FH in the DAPI dye. We estimate that 63 ± 6 pW of the propagated SH average power is required for detectable dye excitation. Finally, we model the waveguiding of the SH light to determine the smallest NW cross-section (around 40x60 nm(2)) which is potentially able to excite fluorescence with a FH intensity below the cell damage threshold.

Far-field imaging for direct visualization of light interferences in GaAs nanowires.

The optical and electrical characterization of nanostructures is crucial for all applications in nanophotonics. Particularly important is the knowledge of the optical near-field distribution for the design of future photonic devices. A common method to determine optical near-fields is scanning near-field optical microscopy (SNOM) which is slow and might distort the near-field. Here, we present a technique that permits sensing indirectly the infrared near-field in GaAs nanowires via its second-harmonic generated (SHG) signal utilizing a nonscanning far-field microscope. Using an incident light of 820 nm and the very short mean free path (16 nm) of the SHG signal in GaAs, we demonstrate a fast surface sensitive imaging technique without using a SNOM. We observe periodic intensity patterns in untapered and tapered GaAs nanowires that are attributed to the fundamental mode of a guided wave modulating the Mie-scattered incident light. The periodicity of the interferences permits to accurately determine the nanowires' radii by just using optical microscopy, i.e., without requiring electron microscopy.