Mid-Infrared Mapping of Four-Layer Graphene Polytypes Using Near-Field Microscopy.

The mid-infrared (MIR) spectral region attracts attention for accurate chemical analysis using photonic devices. Few-layer graphene (FLG) polytypes are promising platforms, due to their broad absorption in this range and gate-tunable optical properties. Among these polytypes, the noncentrosymmetric ABCB/ACAB structure is particularly interesting, due to its intrinsic bandgap (8.8 meV) and internal polarization. In this study, we utilize scattering-scanning near-field microscopy to measure the optical response of all three tetralayer graphene polytypes in the 8.5-11.5 µm range. We employ a finite dipole model to compare these results to the calculated optical conductivity for each polytype obtained from a tight-binding model. Our findings reveal a significant discrepancy in the MIR optical conductivity response of graphene between the different polytypes than what the tight-binding model suggests. This observation implies an increased potential for utilizing the distinct tetralayer polytypes in photonic devices operating within the MIR range for chemical sensing and infrared imaging.

Diffraction-based nonlinear model for the design of broadband adiabatic up-conversion imaging.

In recent years, mid-infrared parametric upconversion imaging, a nonlinear optical method that involves converting mid-infrared light into visible images, has significantly advanced and has shown considerable potential for various applications, including biomedical imaging and remote sensing. While diffraction-based parametric upconversion imaging modeling in standard thin birefringence crystals have been addressed, the numerical framework developed so far fails to address long aperiodic poled crystals. Specifically, diffraction-based analysis of the recent broadband adiabatic frequency upconversion imaging, which allows simultaneous image upconversion of extremely broadband signals is still lacking. Here, we introduce a diffraction-based numerical simulation framework for predicting the evolution of the nonlinear image/signal generation in upconversion imaging systems. This generalized framework can handle both periodically and aperiodically poled crystal designs. Specifically, the model captures faithfully and addresses the varying image magnification arising from upconversion at a Fourier plane of a multiwavelength object. The numerical simulations are validated by experimental measurements of broadband upconversion 3-5 µm mid-IR images to the visible-NIR, showing a good agreement. Moreover, the model allows the exploration of the trade-offs in the spectral span when moving to the full visible range. Our numerical framework will be useful for the interpretation of experimental results obtained in an imaging setting with nonlinear optical elements.

Passively CEP stable sub-2-cycle source in the mid-infrared by adiabatic difference frequency generation.

We report on the generation of a passive carrier-envelope phase (CEP) stable 1.7-cycle pulse in the mid-infrared by adiabatic difference frequency generation. With sole material-based compression, we achieve a sub-2-cycle 16-fs pulse at a center wavelength of 2.7 µm and measured a CEP stability of <190 mrad root mean square. The CEP stabilization performance of an adiabatic downconversion process is characterized for the first time, to the best of our knowledge.

Second-Order Photoinduced Reflectivity for Retrieval of the Dynamics in Plasmonic Nanostructures.

Measuring the change in reflectivity (ΔR) using the traditional pump-probe approach can monitor photoinduced ultrafast dynamics in matter, yet relating these dynamic to physical processes for complex systems is not unique. By applying a simple modification to the classical pump-probe technique, we simultaneously measure both the first and second order of ΔR. These additional data impose new constraints on the interpretation of the underlying ultrafast dynamics. In the first application of the approach, we probe the dynamics induced by a pump laser on the local-surface plasmon resonance (LSPR) in gold nanoantennas. Measurements of ΔR over several picoseconds and a wide range of probe wavelengths around the LSPR peak are followed by data fitting using the two-temperature model. The constraints, imposed by the second-order data, lead us to modify the model and force us to include the contribution of nonthermalized electrons in the early stages of the dynamics.

Spatio-temporal ultrafast pulse shaping at the femtosecond-nanometer scale.

Optical pulse shaping is a fundamental tool for coherent control of the light-matter interaction. While such control enables the measurement of ultrafast temporal dynamics, simultaneous spatiotemporal control is required for studying non-local ultrafast charge dynamics at the nanoscale. However, obtaining accurate spatial control at a sub-wavelength resolution with conventional optical elements poses significant difficulty. Here, we use the spatiotemporal coupling naturally arising in a spatial light modulator based pulse shaping apparatus to achieve accurate control with femto-nano spatiotemporal resolution. We experimentally demonstrate spatial steering at the sub-micron scale of second harmonic generation from nanostructures. In addition, we apply an absolute-value spectral phase to achieve controlled double pulses for nanoscale excitation. We introduce a novel, to the best of our knowledge, scheme for accurate tunable spatiotemporal pump-probe experiments. This method offers rich insight into materials with ultrafast transport phenomena at the femtosecond-nanometer regimes.

Inverse design of unparametrized nanostructures by generating images from spectra.

Recently, there has been an increasing number of studies applying machine learning techniques for the design of nanostructures. Most of these studies train a deep neural network (DNN) to approximate the highly nonlinear function of the underlying physical mapping between spectra and nanostructures. At the end of training, the DNN allows an on-demand design of nanostructures, i.e., the model can infer nanostructure geometries for desired spectra. While these approaches have presented a new paradigm, they are limited in the complexity of the structures proposed, often bound to parametric geometries. Here we introduce spectra2pix, which is a DNN trained to generate 2D images of the target nanostructures. By predicting an image, our model architecture is not limited to a closed set of nanostructure shapes, and can be trained for the design of a much wider space of geometries. We show, for the first time, to the best of our knowledge, a successful generalization ability, by designing completely unseen shapes of geometries. We attribute the successful generalization to the ability of a pixel-wise architecture to learn local properties of the meta-material, therefore mimicking faithfully the underlying physical process. Importantly, beyond synthetical data, we show our model generalization capability on real experimental data.

Robust, efficient, and broadband SHG of ultrashort pulses in composite crystals.

We experimentally demonstrate efficient second-harmonic generation (SHG) of tunable ultrashort pulses of 100 femtoseconds, using a novel method based on composite segmented periodically poled (CSPP) design. The scheme was borrowed from the nuclear magnetic resonance (NMR) composite pulses (CP) of Shaka and Pines. Using CSPP, a broadband and efficient conversion over a bandwidth of 35 nm in very short interaction length was achieved. In addition, CSPP showed robustness to temperature changes up to 90°C. Two CSPP schemes with 15 and 31 segments and periodically poled design were implemented on Mg-doped LiNbO3 crystal. The CSPP performance was shown to be superior in all aspects. The experimental results are compared to numerical simulation with excellent agreement.

High-resolution multi-scan compact Fourier transform-infrared spectrometer.

The Fourier transform-infrared (FT-IR) spectrometer is a widely used high-resolution spectral characterization method in materials, chemicals, and more. However, the inverse relation between the spectral resolution and the interferometer's arm length yields a tradeoff between spectral resolution and spectrometer footprint. Here, we introduce a novel method to overcome this traditional FT-IR resolution limit. The enhanced high-resolution multi-scan compact FT-IR spectrometer we present achieves an effectively long interferogram by combining multiple short FT-IR scans. Simulation and experimental results demonstrate a significant increase in the spectral resolution of a FT-IR spectrometer by employing our interferogram stitching algorithm.

Adiabatic four-wave mixing frequency conversion.

We introduce the concept of adiabatic four-wave mixing (AFMW) frequency conversion in cubic nonlinear media through an analogy to dynamics in quantum two-level systems. Rapid adiabatic passage in four-wave mixing enables coherent near-100% photon number down-conversion or up-conversion over a bandwidth much larger than ordinary phase-matching bandwidths, overcoming the normal efficiency-bandwidth trade-off. We develop numerical methods to simulate AFWM pulse propagation in silicon photonics and fiber platforms as examples. First, we show that with a longitudinally varying silicon waveguide structure, a bandwidth of 70 nm centered at 1820 nm can be generated with 90% photon number conversion. Second, we predict the broadband generation of nanojoule energy, 4.2-5.2 µm mid-infrared light in a short, linearly tapered fluoride step-index fiber. We expect the AFWM concept to be broadly applicable to cubic nonlinear platforms, for applications as diverse as bright ultrafast light pulse generation, sensing, and conversion between telecommunications bands.

Observation of linear plasmonic breathers and adiabatic elimination in a plasmonic multi-level coupled system.

We provide experimental and numerical demonstrations of plasmonic propagation dynamics in a multi-level coupled system, and present the first observation of plasmonic breathers propagating in such systems. The effect is observed both for the simplest symmetric case of a thin metal layer surrounded by two identical dielectrics, and also for a more complex system that includes five and more layers. By a careful choice of the permittivities and thicknesses of the intermediate layers, we can adiabatically eliminate the plasmonic waves in all the intermediate interfaces, thus enabling efficient vertical delivery and extraction of plasmonic signals between the top layer and deeply buried layers. The observation relies on controlling the excited mode by breaking the symmetry of excitation, which is crucial for obtaining the results experimentally. We also observe this breathing effect for transversely shaped plasmonic beams, with Hermite-Gauss, Airy and Weber wavefronts, that despite the oscillatory nature of propagation in such systems, still preserve all their unique wavefront properties. Finally, we show that such approaches can be extended to plasmonic propagation in a general multi-layered system, opening a path for efficient three-dimensional integrated plasmonic circuitry.

Introduction: Nonlinear Optics (NLO) 2017 feature issue.

The editors introduce the feature issue on "Nonlinear Optics 2017," based on the topics presented at the NLO 2017 conference, which was held in Waikoloa, Hawaii, USA from July 17-21, 2017. This feature issue is jointly published by Optics Express and Optical Materials Express.

Pulse shaping of broadband adiabatic SHG from a Ti-sapphire oscillator.

We experimentally demonstrate an efficient broadband second-harmonic generation (SHG) process with a tunable mode-locked Ti:sapphire oscillator. We have achieved a robust broadband and efficient flat conversion of more than 35 nm wavelength by designing an adiabatic aperiodically poled potassium titanyl phosphate crystal. Moreover, we have shown that with such efficient flat conversion, we can shape and control broadband second-harmonic pulses. More specifically, we assign a spectral phase of absolute value and π-step, which allows wavelength tunable intense pump-probe and amplitude modulation of the broadband second-harmonic output. Such spectral phases serve as a proof of concept for other pulse-shaping applications for nonlinear spectroscopy and imaging.

Nonlinear Surface Lattice Resonance in Plasmonic Nanoparticle Arrays.

We study experimentally second-harmonic generation from arrays of split-ring resonators at oblique incidence and find conditions of more than 30-fold enhancement of the emitted second harmonic with respect to normal incidence. We show that these conditions agree well with a nonlinear Rayleigh-Wood anomaly relation and the existence of a surface lattice resonance at the second harmonic. The existence of a nonlinear surface lattice resonance is theoretically confirmed by extending the coupled dipole approximation to the nonlinear case. We further show that the localized surface plasmon modes that collectively contribute to the surface lattice resonance are inherently dark modes that become highly bright due to the collective interaction.

Synthesis of core-shell single-layer MoS2 sheathing gold nanoparticles, AuNP@1L-MoS2.

Nanoparticles, and more specifically gold nanoparticles (AuNPs), have attracted much scientific and technological interest in the last few decades. Their popularity is attributed to their unique optical, catalytic, electrical and magnetic properties when compared with the bulk. However, one of the main problems with AuNPs is their long-term stability. Two-dimensional materials like MoS2 (WS2) are semiconductors that exhibit a combination of properties which make them suitable for electronic, optical and (photo)catalytic devices. Few-layer MoS2 (WS2) nanoparticles (NPs), and in particular single-layer ones, show intriguing optical and electrical properties which are very different from those of the bulk compounds. Here we demonstrate the synthesis of AuNPs sheathed by a single layer of MoS2 (WS2), i.e. a core-shell nanostructure (AuNP@1L-MoS2). The hybrid NPs exhibit optical properties that are different from those of either constituent and are amenable for modulation via their chemistry, offering a myriad of applications.

Predicting nonlinear properties of metamaterials from the linear response.

The discovery of optical second harmonic generation in 1961 started modern nonlinear optics. Soon after, R. C. Miller found empirically that the nonlinear susceptibility could be predicted from the linear susceptibilities. This important relation, known as Miller's Rule, allows a rapid determination of nonlinear susceptibilities from linear properties. In recent years, metamaterials, artificial materials that exhibit intriguing linear optical properties not found in natural materials, have shown novel nonlinear properties such as phase-mismatch-free nonlinear generation, new quasi-phase matching capabilities and large nonlinear susceptibilities. However, the understanding of nonlinear metamaterials is still in its infancy, with no general conclusion on the relationship between linear and nonlinear properties. The key question is then whether one can determine the nonlinear behaviour of these artificial materials from their exotic linear behaviour. Here, we show that the nonlinear oscillator model does not apply in general to nonlinear metamaterials. We show, instead, that it is possible to predict the relative nonlinear susceptibility of large classes of metamaterials using a more comprehensive nonlinear scattering theory, which allows efficient design of metamaterials with strong nonlinearity for important applications such as coherent Raman sensing, entangled photon generation and frequency conversion.

Experimental Realization of Two Decoupled Directional Couplers in a Subwavelength Packing by Adiabatic Elimination.

On-chip optical data processing and photonic quantum integrated circuits require the integration of densely packed directional couplers at the nanoscale. However, the inherent evanescent coupling at this length scale severely limits the compactness of such on-chip photonic circuits. Here, inspired by the adiabatic elimination in a N-level atomic system, we report an experimental realization of a pair of directional couplers that are effectively isolated from each other despite their subwavelength packing. This approach opens the way to ultradense arrays of waveguide couplers for integrated optical and quantum logic gates.

Highly efficient broadband sum-frequency generation in the visible wavelength range.

We report on efficient broadband sum-frequency generation, converting a 140 THz near-infrared bandwidth to the visible regime with photon conversion efficiency greater than 90%. Using a 20-mm-long aperiodically adiabatively poled KTP crystal, the spectral range 660-990 nm was converted to 405-500 nm using a strong pump wave at 1030 nm. The photon conversion efficiency was confirmed to be 92±0.5% when pumped with an intensity of 0.94 GW/cm2. Our experimental results agreed very well with analytic predictions and numerical simulations.

The Short-term Effects of Artificial Tears on the Tear Film Assessed by a Novel High-Resolution Tear Film Imager: A Pilot Study.

PURPOSE: The purpose of this study was to investigate the effects of artificial tears (AT) on the sublayers of the tear film assessed by a novel tear film imaging (TFI) device. METHODS: The mucoaqueous layer thickness (MALT) and lipid layer thickness (LLT) of 198 images from 11 healthy participants, 9 of whom had meibomian gland disease, were prospectively measured before and after exposure to 3 different AT preparations (Refresh Plus; Retaine [RTA]; Systane Complete PF [SYS]), using a novel nanometer resolution TFI device (AdOM, Israel). Participants were assessed at baseline and at 1, 5, 10, 30, and 60 minutes after instilling 1 drop of AT during 3 sessions on separate days. Repeated-measures analysis of variances were used for comparisons with P < 0.05 considered significant. RESULTS: For all ATs, the mean MALT was greatest 1 minute after drop instillation, with an increase of 67%, 55%, and 11% above the baseline for SYS, Refresh Plus, and RTA, respectively. The SYS formulation demonstrated the highest percentage increases in mean MALT and LLT at most postdrop time points. The MALT differences were significantly higher in the SYS than in the RTA (P = 0.014). After 60 minutes, no AT group demonstrated statistically significant changes in MALT or LLT compared with baseline. CONCLUSIONS: We report, for the first time, the effects of AT on MALT and LLT using a high-resolution TFI. A substantial acute mean MALT increase occurs 1 minute after AT instillation with all agents tested, but there were clear differences in response and durability, suggesting the benefits of choosing specific AT according to the needs of each patient.

Octave-spanning coherent mid-IR generation via adiabatic difference frequency conversion.

We demonstrate efficient downconversion of a near-IR broadband optical parametric chirped pulse amplifier (OPCPA) pulse to a 1.1-octave-spanning mid-IR pulse (measured at -10 dB of peak) via a single nonlinearly and adiabatically chirped quasi-phase-matching grating in magnesium oxide doped lithium niobate. We report a spectrum spanning from 2 to 5 µm and obtained by near full photon number conversion of µJ-energy OPCPA pulses spanning 680-870 nm mixed with a narrowband 1047-nm pulse. The conversion process is shown to be robust for various input broadband OPA pulses and suitable for post-amplification conversion for many near-IR systems.

Rayleigh anomaly induced phase gradients in finite nanoparticle chains.

Collective optical interactions in infinite nanoparticle arrays have been studied intensively over the past decade. However, analysis of finite arrays has received significantly less attention. Here, we theoretically and numerically show that the collective interaction in finite nanoparticle chains can support phase gradients that shift the diffraction pattern with respect to infinite chains. Specifically, we demonstrate that this phenomenon occurs for resonating nanoparticles in a narrow spectral range around the Rayleigh anomaly condition, i.e., when a certain diffraction order radiates at a grazing angle. This reveals that the Rayleigh anomaly, which is associated with intensity changes, can also induce angular anomalies in finite arrays. To study the effect theoretically, we develop a novel analytical approach based on the discrete dipole approximation. Within this framework, we find an approximate closed-form solution to the particles' dipole moments. We show that our solution can be expressed in two different ways, one based on a combinatorial calculation, and the other on a recursive calculation, and discuss the unique physical interpretation emerging from each of them. Our results are of potential importance in a wide range of practical applications from LIDARs to beam shaping schemes.