Nonlinear Frequency Upconversion Research Articles

Harnessing nonlinear frequency upconversion of Talbot effect with flexible Talbot lengths

We report on a simple experimental scheme demonstrating nonlinear frequency upconversion of the Talbot effect with controllable Talbot lengths at high conversion efficiency. Using a microlens array (MLA) as an array illuminator at 1064 nm onto a 1.2-mm-thick BiBO crystal, we have observed the second harmonic Talbot effect in green at 532 nm with a Talbot length twice that of the pump Talbot length. However, the Talbot length is constant for fixed parameters of the periodic object and the laser wavelength. With the formulation of a suitable theoretical framework, we have implemented a generic experimental scheme based on the Fourier transformation technique to independently control the Talbot lengths of the MLA in both the pump and the second harmonic, overcoming the stringent dependence of MLA parameters on the self-images. Deploying the current technique, we have been able to tune the Talbot lengths from z T = 26 cm to z T = 62.4 cm in the pump and z T = 12.4 cm to z T = 30.8 cm in the second harmonic, respectively. The single pass conversion efficiency of the Talbot images is 2.91% W−1, an enhancement of a factor of 106 as compared to the previous reports. This generic experimental scheme can be used to generate long-range self-images of periodic structures and also to program desired Talbot planes at required positions at both pump and upconverted frequency to avoid any mechanical constraints of experiments.

Generation of high-energy, sub-20 fs deep-UV pulses in a twin-crystal third harmonic generation scheme.

Ultrashort deep ultraviolet (DUV) pulses serve as indispensable tools for investigating molecular dynamics on the femtosecond scale. Nonlinear frequency upconversion of near-infrared (NIR) light sources in a sequence of nonlinear crystals is a common method for their generation. However, preserving the temporal duration of the starting source encounters challenges owing to phase-matching bandwidth limitations within the harmonic generation process. Here we propose an approach for circumventing this limitation and demonstrate it for the case of generation of the third harmonic of 800 nm pulses in a two-stage scheme (second harmonic generation succeeded by sum-frequency mixing of the fundamental and second harmonic pulses). Expanding the bandwidth of the DUV pulse involves the utilization for the last mixing process of two nonlinear crystals, detuned to convert opposite sides of the spectrum. The implementation of this approach yields 20 µJ, 263 nm DUV pulses as short as 19 fs after compression. The setup is very compact and extremely stable due to the common-path scheme, which makes it very interesting for a variety of advanced ultrafast spectroscopy applications.

Nonlinear frequency up-conversion of perfect vortex beams based on four wave-mixing in 85Rb atoms

Optical vortices are widely explored in quantum optics and communication because of their quantized orbital angular momentum, especially its applications in the frequency conversion process lay a foundation for establishing frequency interfaces. However, limited by the spatial mode matching, constructing the frequency interfaces with uniform conversion efficiency is still a challenge. Here, we propose and demonstrate a frequency up-conversion of perfect vortex beams for accommodating arbitrary topological charges in a diamond atomic system of 85Rb. In this process, the 780 nm, 776 nm and internally generated 5233 nm light fields induce the 420 nm coherent blue light generation. The 776 nm perfect vortex beam with transverse structure-invariance serves as the signal beam, which leads to the uniform conversion efficiency and is accompanied by orbital angular momentum transfer of output 420 nm coherent blue light. In addition, in view of the tunable radius and width, the perfect vortex beams with different transverse sizes are also successfully transferred, which further increases the encoding flexibility.

Mid-infrared single-photon 3D imaging

Active mid-infrared (MIR) imagers capable of retrieving three-dimensional (3D) structure and reflectivity information are highly attractive in a wide range of biomedical and industrial applications. However, infrared 3D imaging at low-light levels is still challenging due to the deficiency of sensitive and fast MIR sensors. Here we propose and implement a MIR time-of-flight imaging system that operates at single-photon sensitivity and femtosecond timing resolution. Specifically, back-scattered infrared photons from a scene are optically gated by delay-controlled ultrashort pump pulses through nonlinear frequency upconversion. The upconverted images with time stamps are then recorded by a silicon camera to facilitate the 3D reconstruction with high lateral and depth resolutions. Moreover, an effective numerical denoiser based on spatiotemporal correlation allows us to reveal the object profile and reflectivity under photon-starving conditions with a detected flux below 0.05 photons/pixel/second. The presented MIR 3D imager features high detection sensitivity, precise timing resolution, and wide-field operation, which may open new possibilities in life and material sciences.

High‐Speed Mid‐Infrared Single‐Photon Upconversion Spectrometer

AbstractSensitive and fast mid‐infrared (MIR) spectroscopy is highly attractive in a variety of applications including astronomical observation, pharmaceutical synthesis, and environmental monitoring. However, the performance of conventional MIR spectrometers has long been hindered by the limited sensitivity of narrow‐bandgap detectors and/or the deficient brightness of broadband light sources. Here, an ultra‐sensitive and broadband MIR upconversion spectrometer, which integrates a supercontinuum source covering 1.5–4.2 m based on a silicon nitride nanophotonic waveguide, is devised and integrated. High‐efficiency and low‐noise nonlinear frequency upconversion is realized based on coincidence pulsed pumping with spectro‐temporal optimization, which enables leverage of silicon detectors for facilitating MIR single‐photon spectroscopy at 0.2 photons/nm/pulse. Furthermore, the upconversion‐based array spectrometer is manifested with high‐speed spectral acquisition rates beyond 200 kHz, which is about tenfold faster than the state‐of‐the‐art scan rates for FTIR‐based spectrometers at a comparable spectral resolution. The achieved features of broadband spectral coverage, single‐photon sensitivity, and sub‐MHz refreshing rate might open up new possibilities for infrared transient spectral measurements in combustion analysis, high‐throughput sorting, and reaction tracking, among others.

Mid‐Infrared Single‐Photon Edge Enhanced Imaging Based on Nonlinear Vortex Filtering

AbstractEdge enhanced imaging via the spiral phase contrast enables to reveal the phase or amplitude gradients of a target, which has been proved useful in feature recognition, machine vision, and object identification. A long quest is to extend the operation wavelength into the mid‐infrared (MIR) region, as highly demanded in various fields including infrared sensing, astronomic observation, and biomedical diagnosis. Here, ultra‐sensitive MIR imaging at the single‐photon level based on nonlinear frequency upconversion is demonstrated, where the spectrally converted replica of the MIR object image at 3070 nm is captured by a silicon electron multiplying charged coupled device. The imaging sensitivity is significantly improved by the coincidence pulsed pumping with a spectro‐temporal optimization. Furthermore, the edge enhancement is realized by imprinting the spiral phase pattern of the pump onto the upconverted field at the Fourier plane within the nonlinear crystal. Such a nonlinear spatial filter not only provides an effective way to implement the required high‐fidelity vortex screening in the edge enhanced detection, but also renders the MIR illumination into a visible image in an efficient and low‐noise fashion. The presented system for MIR edge enhanced imaging might facilitate immediate applications in label‐free histopathological diagnosis and non‐destructive defect inspection.

Low noise frequency upconversion imaging based on Hadamard coding and time-gate detection

The nonlinear frequency upconversion with the tight focused pump beam based on photon counting and Hadamard coding is presented to acquire low noise converted images. The pump beam is optimized by tight focusing to enhance its power density in nonlinear crystal. In order to reduce the distortion caused by the point spread function effect, the object is encoded by measurement matrices and the converted photons corresponding to each pattern is measured. Thus the converted image with sharp edges can be reconstructed by the measurements and the measurement matrices. The time-gated detection is applied to increase the signal-to-noise ratio(SNR) of the measurements. The experimental results show the peak of the dark noise is less than 0.34 photons/spatial/s element for an image with 64 × 64 pixels by taking into account 10 ms measurement time for each pattern. Compared with the converted image reconstructed by the measurements of the photomultiplier tube(PMT) directly, the peak signal to noise ratio (PSNR) of photon counting image increases about 30.91%.

Theoretical Exploration of Terahertz Single-Photon Detection and Imaging by Nonlinear Optical Frequency Up-Conversion

Terahertz single-photon detection and imaging have attracted full attention recently. Nonlinear optical frequency up-conversion is a promising technique that can be expected to satisfy this demand thanks to its high sensitivity and fast response. In this paper, theoretical analysis and numerical calculations based on the organic salt 4′-dimethylamino-N-methyl-4-stilbazolium tosylate (DAST) crystal were performed to show that the optimization of the detection of terahertz is different from that of the generation of terahertz, including the use of difference-frequency generation (DFG) technique, the larger thickness of the crystal, and especially the selection of the polarization direction of the pumping laser. For two different polarization configurations, the photons of the up-converted signal light both can be amplified compared with the number of incident terahertz photons under some optimal designs of the nonlinear frequency conversion process. Therefore, terahertz single-photon detection can be realized with single-photon detectors (SPDs) or even possibly with ordinary avalanche photodiodes (APDs). Furthermore, for terahertz single-photon imaging, the frequency up-conversion with the pumping laser polarized along b-axis of DAST crystal has a better performance, which is rarely used in terahertz generation.

Up-Conversion Imaging Processing With Field-of-View and Edge Enhancement

Spiral phase contrast is an important and convenient imaging processing technology in edge detection, and a broader field-of-view (FOV) of imaging is a long-pursuing aim to see more regions of the illumination objects. Compared with near-infrared (NIR) spectrum, the up-conversion imaging in visible spectrum benefits from the advantages of higher efficiency detection and lower potential speckle. FOV enhanced and spiral phase contrast up-conversion imaging processing methods by using second order nonlinear frequency up-conversion from NIR spectrum to visible spectrum in two different configurations are presented in this work. By changing the temperature of crystal, controllable spatial patterns of imaging with more than 4.5 times enhancement of FOV is realized in both configurations. Additionally, we present numerical simulations of the phenomenon, which agree well with the experimental observations. Our results provide a very promising way in imaging processing, which may be widely used in biomedicine, remote sensing and up-conversion monitoring.

Nonlinear frequency conversion in one dimensional lithium niobate photonic crystal nanocavities

We demonstrate flexible nonlinear frequency up-conversion in high-Q lithium niobate photonic crystal nanobeam resonators. The high optical Q together with strong optical mode confinement allows us to observe clear second harmonic generation and sum frequency generation with an optical power around only tens of microWatts. These demonstrations show that high-Q lithium niobate photonic crystal nanoresonators are of great promise for nonlinear photonic applications.

On-the-Fly Control of High-Harmonic Generation Using a Structured Pump Beam.

We demonstrate experimentally a relatively simple yet powerful all-optical enhancement and control technique for high harmonic generation. This is achieved by using as a pump beam two different spatial optical modes interfering together to realize tunable periodic quasi-phase matching of the interaction. With this technique, we demonstrate on-the-fly quasi-phase matching of harmonic orders 29-41 at ambient gas pressure levels of 50 and 100 Torr, where an up to 100-fold enhancement of the emission is observed. The technique is scalable to different harmonic orders and ambient pressure conditions.

Nonlinear frequency up-conversion via double topological edge modes.

We study the nonlinear frequency up-conversion in a plasmonic thin film sandwiched between one-dimensional photonic crystals (PCs) of different Zak phases by rigorous numerical time-domain nonlinear hydrodynamic calculations. We show that the proposed hetero-structure can support robust fundamental and high-order topological edge modes that simultaneously enhance the third-harmonic generation. Numerical simulations also show that femtosecond pulses can excite double topological edge modes through optical tunneling in band gaps, leading to a large nonlinear response. The obtained third harmonic generation (THG) conversion efficiency of the hetero-structure is three orders of magnitude larger than that of a single plasmonic film. The results presented here may open new avenues for designing high-efficiency nonlinear photonic devices.

Mid-infrared upconversion based hyperspectral imaging.

Mid-infrared hyperspectral imaging has in the past decade emerged as a promising tool for medical diagnostics. In this work, nonlinear frequency upconversion based hyperspectral imaging in the 6 to 8 µm spectral range is presented for the first time, using both broadband globar and narrowband quantum cascade laser illumination. AgGaS2 is used as the nonlinear medium for sum frequency generation using a 1064 nm mixing laser. Angular scanning of the nonlinear crystal provides broad spectral coverage at every spatial position in the image. This study demonstrates the retrieval of series of monochromatic images acquired by a silicon based CCD camera, using both broadband and narrowband illumination and a comparison is made between the two illumination sources for hyperspectral imaging.

An experimentally validated model for geometrically nonlinear plucking-based frequency up-conversion in energy harvesting

It is well known that plucking-based frequency up-conversion can enhance the power output in piezoelectric energy harvesting by enabling cyclic free vibration at the fundamental bending mode of the harvester even for very low excitation frequencies. In this work, we present a geometrically nonlinear plucking-based framework for frequency up-conversion in piezoelectric energy harvesting under quasistatic excitations associated with low-frequency stimuli such as walking and similar rigid body motions. Axial shortening of the plectrum is essential to enable plucking excitation, which requires a nonlinear framework relating the plectrum parameters (e.g. overlap length between the plectrum and harvester) to the overall electrical power output. Von Kármán-type geometrically nonlinear deformation of the flexible plectrum cantilever is employed to relate the overlap length between the flexible (nonlinear) plectrum and the stiff (linear) harvester to the transverse quasistatic tip displacement of the plectrum, and thereby the tip load on the linear harvester in each plucking cycle. By combining the nonlinear plectrum mechanics and linear harvester dynamics with two-way electromechanical coupling, the electrical power output is obtained directly in terms of the overlap length. Experimental case studies and validations are presented for various overlap lengths and a set of electrical load resistance values. Further analysis results are reported regarding the combined effects of plectrum thickness and overlap length on the plucking force and harvested power output. The experimentally validated nonlinear plectrum–linear harvester framework proposed herein can be employed to design and optimize frequency up-conversion by properly choosing the plectrum parameters (geometry, material, overlap length, etc) as well as the harvester parameters.

Asymmetric Nanocrescent Antenna on Upconversion Nanocrystal.

Frequency upconversion activated with lanthanide has attracted attention in various real-world applications, because it is far simpler and more efficient than traditional nonlinear susceptibility-based frequency upconversion, such as second harmonic generation. However, the quantum yield of frequency upconversion of lanthanide-based upconversion nanocrystals remains inefficient for practical applications, and spatial control of upconverted emission is not yet developed. Here, we developed an asymmetric nanocrescent antenna on upconversion nanocrystal (ANAU) to deliver excitation light effectively to the core of upconversion nanocrystal by nanofocusing light and generating asymmetric frequency upconverted emission concentrated toward the tip region. ANAUs were fabricated by high-angle deposition (60°) of gold (Au) on the isolated upconversion nanoparticles supported by nanopillars then moved to refractive-index matched substrate for orientation-dependent upconversion luminescence analysis in the single-nanoparticle scale. We studied shape-dependent nanofocusing efficiency of nanocrescent antennae as a function of the tip-to-tip distance by modulating the deposition angle. The generation of asymmetric frequency upconverted emission toward the tip region was simulated by the asymmetric far-field radiation pattern of dipoles in the nanocrescent antenna and experimentally demonstrated by the orientation-dependent photon intensity of frequency upconverted emission of an ANAU. This finding provides a new way to improve frequency upconversion using an antenna, which locally increases the excitation light and generates the radiation power to certain directions for various applications.

Low Frequency Vibration Energy Harvester Using Stopper-Engaged Dynamic Magnifier for Increased Power and Wide Bandwidth

We present a piezoelectric energy harvester with stopper-engaged dynamic magnifier which is capable of significantly increasing the operating bandwidth and the energy (power) harvested from a broad range of low frequency vibrations (<30 Hz). It uses a mass-loaded polymer beam (primary spring-mass system) that works as a dynamic magnifier for another mass-loaded piezoelectric beam (secondary spring-mass system) clamped on primary mass, constituting a two-degree-of-freedom (2-DOF) system. Use of polymer (polycarbonate) as the primary beam allows the harvester not only to respond to low frequency vibrations but also generates high impulsive force while the primary mass engages the base stopper. Upon excitation, the dynamic magnifier causes mechanical impact on the base stopper and transfers a secondary shock (in the form of impulsive force) to the energy harvesting element resulting in an increased strain in it and triggers nonlinear frequency up-conversion mechanism. Therefore, it generates almost four times larger average power and exhibits over 250% wider half-power bandwidth than those of its conventional 2-DOF counterpart (without stopper). Experimental results indicate that the proposed device is highly applicable to vibration energy harvesting in automobiles.

The role of ferroelectric domain wall in nonlinear Cerenkov frequency up-conversion in 1D nonlinear crystal

We reveal a variety of nonlinear Cerenkov radiation (NCR) patterns that occur in a single photonic crystal modulated by domain walls, which manifest themselves as normal, degenerated, and anomalous-dispersion-like NCR type sum-frequency generation. The phase-matching geometries of the evolution of Cerenkov radiation varying with the dispersion relationship among the interaction waves are exploited, respectively.

Infrared hyperspectral upconversion imaging using spatial object translation.

In this paper hyperspectral imaging in the mid-infrared wavelength region is realised using nonlinear frequency upconversion. The infrared light is converted to the near-infrared region for detection with a Si-based CCD camera. The object is translated in a predefined grid by motorized actuators and an image is recorded for each position. A sequence of such images is post-processed into a series of monochromatic images in a wavelength range defined by the phasematch condition and numerical aperture of the upconversion system. A standard USAF resolution target and a polystyrene film are used to impart spatial and spectral information unto the source.

Piezoceramic based wideband energy harvester using impact-enhanced dynamic magnifier for low frequency vibration

Piezoceramic materials (such as PZT) have excellent piezoelectric properties and have been extensively used in vibration energy harvesting. Conventional piezoceramic-based energy harvesters (SDOF systems) are only efficient near their 1st resonance, and their 2nd resonance is generally ignored due to the higher frequency and comparatively lower response level. A properly designed dynamic magnifier can be used in a 2-DOF system to increase the effective bandwidth of the device by reducing the frequency gap between the 1st and 2nd resonances. The output is therefore improved by increasing the strain produced in the piezoelectric cantilever. Nevertheless, such a device cannot effectively harvest energy from vibrations at a frequency below 30Hz. We present a piezoceramic-based wideband low-frequency vibration energy harvester that exploits the mechanical impact of the mass of a flexible dynamic magnifier on a harvester base stopper. This mechanical impact delivers a large secondary force to a piezoceramic cantilevered secondary beam, resulting in an increased strain and also triggering a non-linear frequency up-conversion mechanism that increases both the output power and the bandwidth of the operating frequency. A prototype energy harvester with a mass ratio of μ=5.8 and a stopper distance of d=0.5mm generated a peak power with a maximum of 449μW delivered to an optimal load of 30kΩ at a frequency of 17Hz, and the half-power bandwidth was found to be 15Hz (from 9Hz to 24Hz) at 1g of acceleration, indicating that the device is capable of efficiently harvesting energy from a broad range of low-frequency random vibrations as well as shocks.

Diffraction-limited real-time terahertz imaging by optical frequency up-conversion in a DAST crystal.

Real-time terahertz (THz) wave imaging has wide applications in areas such as security, industry, biology, medicine, pharmacy, and the arts. This report describes real-time room-temperature THz imaging by nonlinear optical frequency up-conversion in an organic 4-dimethylamino-N'-methyl-4'-stilbazolium tosylate (DAST) crystal, with high resolution reaching the diffraction limit. THz-wave images were converted to the near infrared region and then captured using an InGaAs camera in a tandem imaging system. The resolution of the imaging system was analyzed. Diffraction and interference of THz wave were observed in the experiments. Videos are supplied to show the interference pattern variation that occurs with sample moving and tilting.