Nonlinear Frequency Conversion Research Articles

Nonlinear generation of vector beams by using a compact nonlinear fork grating

Vectorial beams have attracted great interest due to their broad applications in optical micromanipulation, optical imaging, optical micromachining, and optical communication. Nonlinear frequency conversion is an effective technique to expand the frequency range of the vectorial beams. However, the scheme of existing methods to generate vector beams of the second harmonic (SH) lacks compactness in the experiment. Here, we introduce a new way to realize the generation of vector beams of SH by using a nonlinear fork grating to solve such a problem. We examine the properties of generated SH vector beams by using Stokes parameters, which agree well with theoretical predictions. Then we demonstrate that linearly polarized vector beams with arbitrary topological charge can be achieved by adjusting the optical axis direction of the half-wave plate (HWP). Finally, we measure the nonlinear conversion efficiency of such a method. The proposed method provides a new way to generate vector beams of SH by using a microstructure of nonlinear crystal, which may also be applied in other nonlinear processes and promote all-optical waveband applications of such vector beams.

Transmission and nanohardness studies of ternary GaAs1-xPx layers grown from the vapor phase by heteroepitaxy

Transmission measurements in the 0.5–25-μm spectral range are performed on thin (<350 -μm) GaAsP layers grown by Hydride Vapor Phase Epitaxy (HVPE) on plain (100) GaAs substrates. Comparison with calculations taking into account multiple reflections reveals the role of the surface polishing quality on the clear transmission window and the wavelength dependent losses. A measurement of a 5-mm thick epitaxially grown GaP underlines more realistic spectral limitations on the application of orientation-patterned structures based on GaP and GaAsP for nonlinear optical frequency conversion. The mid-IR cut-off wavelength for the ternary GaAsP layers is almost independent of the composition and corresponds to the same two-phonon absorption limit observed in the binary GaP. Nanohardness and Young's modulus are measured for the same samples to evaluate their compositional dependence. The nanohardness dependence on the P-content obeys a second order polynomial law with a maximum around P = 0.8. Young's modulus depends linearly on the P-content, similar to the trend observed in other ternary systems, such as InxGa1−xAs and InxGa1-xP. The evolution of the band-gap, estimated from the transmission measurements, with the composition of the ternary compounds is linear in the range of 0–0.5 for the P content. In this same range the nanohardness can be considered to be linearly proportional to the band-gap.

High-efficiency anti-stokes Raman blue laser in CO2 enables high-luminance RGB laser-driven white light

Stimulated Raman scattering (SRS) is an efficient nonlinear frequency conversion method, enabling simultaneous generation of red, green, and blue (RGB) lasers. In order to synthesize a white light source for laser display by SRS, a 532 nm laser was used as pump source, and high purity gaseous carbon dioxide (CO2) was used as the Raman active medium. First, by optimizing experimental parameters, with an f = 1.5 m focal lens, in 0.8 atm CO2 pumped at 304 mJ, a first-order anti-Stokes (AS1) 495 nm blue laser was achieved, with an energy of 31.9 mJ, peak power of 10.9 MW and conversion efficiency (CE) of 10.5 %. Then, Then, the second-order Stokes light (S2) at 624 nm, residual pump laser (S0) at 532 nm, and AS1 laser were utilized as RGB primary colors. By the variation of pressure below 1 atmosphere (atm), the laser-driven white light (LDWL) with adjustable correlated color temperature (CCT) below 4700 K were simulated. Finally, LDWL up to 2.6 × 1018cd/m2 of a CCT of 3300 K could be synthesized at an RGB power ratio of PR: PG: PB = 0.447:0.094:0.459, resulting in a white light power CE of 44.4 % and luminous efficacy of 113.7 lm/W. In addition, use of the 574 nm yellow Raman light is expected to realize a four-primary (RGBY) laser display scheme with higher Luminance and broader color gamut. Moreover, the feasibility of using a 515 nm Yb: YAG laser as pump source to widen the range of CCT and improve the brightness of LDWL was discussed.

Magnetic modes for enhancing second harmonic generation at ultraviolet frequencies

Enhancing nonlinear frequency conversions at ultraviolet (UV) frequencies holds immense significance in contemporary physics and nanophotonics. In this work, we have theoretically demonstrated a highly efficient UV second-harmonic generation (SHG) in the Al nanorod−LiNbO3 (LN)−Al film nanostructure by two orders of magnitude higher compared to the conventional LiNbO3 nanostructure in this range. This result is acquired by designing a simple Al nanoparticle-Al film plasmonic system that generates magnetic resonances at near-UV frequencies to confine light to the LN, which can highly enhance the electromagnetic field and lead to strong interactions with the large nonlinear susceptibility. Our research provides profound insights into the pivotal role of plasmon-induced magnetic resonance (PIMR) modes in UV-SHG processes, thereby opening up new avenues for the development of nanoscale UV nanosources and nonlinear metasurface applications at subwavelength scale.

Frequency converting and digital modulation of light derived from lanthanide for signal encoding and logic computing

AbstractModulation of light underpins a central part of modern optoelectronics. Conventional optical modulators based on refractive‐index and absorption variation in the presence of an electric field serve as the workhorse for diverse photonic technologies. However, these approaches based on electro‐refraction or electro‐absorption effect impose limitations on frequency converting and signal amplification. Lanthanide‐activated phosphors offer a promising platform for nonlinear frequency conversion with an abundant spectrum. Here, we propose a novel approach to achieve frequency conversion and digital modulation of light signal by coupling lanthanide luminescence with an electrically responsive ferroelectric host. The technological benefits of such paradigm‐shifting solution are highlighted by demonstrating a quasi‐continuous and enhancement of the lanthanide luminescence. The ability to locally manipulate light emission can convert digital information signals into visible waveforms, and visualize electrical logic and arithmetic operations. The proof‐of‐concept device exhibits perspectives for developing light‐compatible logic functions. These results pave the way to design more controllable lanthanide photonics with desired opto‐electronic coupling.image

Subwavelength Photorefractive Grating in a Thin‐Film Lithium Niobate Microcavity

AbstractSubwavelength gratings play a fundamental and pivotal role in numerous science and applications for wave manipulation, exhibiting distinctive features such as filtering, phase manipulation, and anti‐reflection. However, conventional fabrication methods for ultrasmall periodic structures are constrained by the fundamental optical diffraction limit, making it challenging to produce subwavelength gratings for optics. Here, a novel technique is demonstrated to build a reconfigurable subwavelength photorefractive grating (SPG) in a thin‐film lithium niobate on the platform of an optical microcavity. Such SPGs are optically induced through the photorefractive effect and the subwavelength features originate from the spatial phase modulations of the pump's standing wave. The resulting SPGs lead to the mode splitting of two counter‐propagating modes inside the microcavity, exhibiting an Electromagnetically Induced Transparency (EIT)‐like transmission spectrum. Moreover, the unique subwavelength characteristic of SPGs enables first‐order quasi‐phase‐matching for backward second‐harmonic generation, a long‐standing problem in nonlinear optics. Also, free‐space‐to‐chip vertical nonlinear frequency conversion can be achieved in a similar manner. These results provide a flexible approach toward fabricating subwavelength gratings, which holds significant potential in various applications such as nonlinear frequency conversion, optical communication, sensing, and quantum technologies.

Sum and difference frequency generation in a valley-photonic-crystal-like topological system

Nonlinear sum frequency generation (SFG) and difference frequency generation (DFG) are fundamental methods to obtain new light sources for various applications. However, most of the on-chip SFG and DFG are based on conventional resonators, lacking robustness against fabrication defects. Here, we demonstrate topologically protected SFG and DFG in a second-order topological photonic system. The mechanism is based on the nonlinear interaction between three high-Q corner modes inside dual topological band gaps. The frequency matching condition for SFG and DFG is precisely satisfied by designing a valley-photonic-crystal-like topological system, which provides more freedoms to tune the corner modes. The topological SFG and DFG are achieved with high conversion efficiency, and the underlying topological physics is revealed. This work opens up avenues toward topologically protected nonlinear frequency conversion, and can find applications in the fields of on-chip single-photon detections and optical quantum memories with robustness against defects.

Near-unity asymmetric transmission of linearly polarized light with high Q-factor based on the coherent coupling of dual resonances in bilayer dielectric chiral metasurfaces

This report shows that near-unity asymmetric transmission (AT) of linearly polarized light with high Q-factor can be realized in bilayer dielectric chiral metasurfaces, the unit cell of which consists of silicon slab with rectangular holes on its both sides which are arranged perpendicularly to each other. The preceding work has revealed that the theoretical upper limit of the AT is given as the amplitude reflection coefficient of background system without nanostructure, when a single resonance mainly contributes. If double resonances with overlapping spectral shapes concurrently contribute to the AT, however, their coherent coupling enables breaking the above upper limit and near-unity AT can be obtained. As one of the contributing resonances in the metasurface is quasi-BIC, the resultant AT has also high Q-factor in addition to the near-unity value. Thus, the presented photonic system exhibits highly efficient asymmetric third-harmonic generation behavior, which has the efficiency ratio between forward and backward pumping in the orders from several hundreds to thousands. High-Q near-unity AT shown in this work will find practical applications for direction-dependent nonlinear frequency conversion, information processing, optical sensing, and polarization multiplexing.

Optical second harmonic generation in anisotropic multilayers with complete multireflection of linear and nonlinear waves using ♯SHAARP.ml package

Optical second harmonic generation (SHG) is a nonlinear optical effect widely used for nonlinear optical microscopy and laser frequency conversion. Closed-form analytical solution of the nonlinear optical responses is essential for evaluating materials whose optical properties are unknown a priori. A recent open-source code, ♯SHAARP.si, can provide such closed form solutions for crystals with arbitrary symmetries, orientations, and anisotropic properties at a single interface. However, optical components are often in the form of slabs, thin films on substrates, and multilayer heterostructures with multiple reflections of both the fundamental and up to ten different SHG waves at each interface, adding significant complexity. Many approximations have therefore been employed in the existing analytical approaches, such as slowly varying approximation, weak reflection of the nonlinear polarization, transparent medium, high crystallographic symmetry, Kleinman symmetry, easy crystal orientation along a high-symmetry direction, phase matching conditions and negligible interference among nonlinear waves, which may lead to large errors in the reported material properties. To avoid these approximations, we have developed an open-source package named Second Harmonic Analysis of Anisotropic Rotational Polarimetry in Multilayers (♯SHAARP.ml). The reliability and accuracy are established by experimentally benchmarking with both the SHG polarimetry and Maker fringes using standard and commonly used nonlinear optical materials as well as twisted 2-dimensional heterostructures.

Broadband long-wavelength upconversion in ultra-short nonlinear crystals.

Since the inception of the second-order nonlinear frequency conversion in 1961, enhancing the inherent low conversion efficiency has been a primary objective. This goal has been successfully accomplished through the utilization of cm-long nonlinear crystals characterized by high quality and nonlinearity, coupled with versatile phase-matching strategies and high-power mixing lasers. However, the reliance on lengthy nonlinear crystals and the necessity for precise phase-matching introduce stringent tolerances on acceptance angles and spectral bandwidths for the interacting fields, thereby constraining its widespread applicability in scientific and industrial domains. This challenge is addressed by combining a broadly tunable ∼5 mW quantum cascade laser operating in the 9.5-12.5 µm range with upconversion detection in ∼100 µm long AGS crystals. Using a tightly focused continuous wave Nd:YVO4 laser with 20 mW output power and spatial filtering of the upconverted beam lead to a SNR of 55 for 50 µs averaging time sufficient for many applications.

Consideration of non-phase-matched nonlinear effects in the design of quasi-phase-matching crystals for optical parametric oscillators.

Femtosecond optical parametric oscillators (OPOs) are widely used in ultrafast nonlinear frequency conversion and quantum information. However, conventional OPOs based on quasi-phase-matching (QPM) crystals have many parasitic non-phase-matched processes which decrease the conversion efficiency. Here, we propose nine-wave coupled equations (NWCEs) to simulate all phase-matched and non-phase-matched interactions in QPM crystals to improve conventional three-wave coupled equations (TWCEs), especially for the situation of high intensity ultrashort pulses and complexly structured crystals. We discuss how to design the poling period of QPM crystal to maximize the conversion efficiency of signal light for a given OPO system. The simulation reveals that the OPO based on chirped periodically poled lithium niobate (CPPLN) with a certain chirp rate has higher signal wave conversion efficiency than that of a PPLN, and demonstrates that NWCEs illustrate more details of the pulse evolution in the OPO cavity. Starting from a CPPLN, an aperiodically poled lithium niobate (APPLN) design is available by modifying the domain lengths of the crystal and optimizing the OPO output power via dynamical optimization algorithm. The results show that by using a properly designed APPLN crystal, a 1600 nm OPO, when pumped by a femtosecond laser with 1030 nm central wavelength, 150 femtosecond pulse duration and 5 GW/cm2 power intensity at the focus, can achieve very efficient output with a signal light conversion efficiency of 50.6%, which is higher than that of PPLN (25.2%) and CPPLN (40.2%). The scheme in this paper will provide a reference for the design of nonlinear QPM crystals of OPOs and will help to understand the complex nonlinear dynamical behavior in OPO cavities.

Nonlinear frequency conversion of nondiffracting modes via nondegenerate four-wave mixing in atomic vapor

Nonlinear frequency conversion of nondiffracting modes via nondegenerate four-wave mixing in atomic vapor

Recent advances in high-order harmonic generation from laser-ablated plumes at the advanced laser light source laboratory

High-order harmonic generation is a nonlinear optical frequency conversion process that occurs during intense ultrafast laser-matter interaction. At the Advanced Laser Light Source laboratory, we use ultrafast laser pulses having diverse wavelengths, spanning visible, near- and mid-infrared ranges, to generate high-order harmonics from laser-ablated plumes in the extreme ultraviolet or soft X-ray region of the electromagnetic spectrum. The Advanced Laser Light Source Laboratory is situated within the Énergie Matériaux Télécommunications Center of the Institut national de la recherche scientifique in Montréal, Quebec, Canada. We focus on generating bright and broadband harmonics by exploiting various types of ultrafast resonances in different species within the laser-ablated plume, and use them for applications in ultrafast spectroscopy, imaging, and AMO science. We are also actively exploring previously unknown physics governing the harmonic generation from different resonances. In this review article, we provide an overview of the recent advancements made in these directions.

Second‐Harmonic Generation with a 440 000% W−1 Conversion Efficiency in a Lithium Niobate Microcavity without Periodic Poling

AbstractThin‐film lithium niobate (TFLN) enables extremely high‐efficiency second‐order nonlinear optical effects due to large nonlinear coefficient d33 and strong optical field confinement. Here, a pulley‐waveguide‐coupled microring resonator with an intrinsic quality factor above 9.4 × 105 on the reverse‐polarized double‐layer X‐cut TFLN is designed and fabricated. In such a TFLN resonator without fine domain structures, second harmonic generation with a normalized conversion efficiency of 440,000% W−1 with weak pump power, approaching that in periodically poled lithium niobate (PPLN) microring resonators, and an absolute conversion efficiency of 30% is realized with a sub‐milliwatt continuous pump. This work reduces the dependence of high‐efficiency nonlinear frequency conversion on PPLN microcavities that are difficult to prepare.

Selective excitation of high-order modes in two-dimensional cavity resonator integrated grating filters.

The selective spatial mode excitation of a bi-dimensional grating-coupled micro-cavity called a cavity resonator integrated grating filter (CRIGF) is reported using an incident beam shaped to reproduce the theoretical emission profiles of the device in one and subsequently two dimensions. In both cases, the selective excitation of modes up to order 10 (per direction) is confirmed by responses exhibiting one (respectively two) spectrally narrowband resonance(s) with a good extinction of the other modes, the latter being shown to depend on the parity and order(s) of the involved modes. These results pave the way toward the demonstration of multi-wavelength spatially selective reflectors or fiber-to-waveguide couplers. Also, subject to an appropriate choice of the materials constituting the CRIGF, this work can be extended to obtain mode-selectable laser emission or nonlinear frequency conversion.

Near-ultraviolet photon-counting dual-comb spectroscopy

Ultraviolet spectroscopy provides unique insights into the structure of matter with applications ranging from fundamental tests to photochemistry in the Earth’s atmosphere and astronomical observations from space telescopes1–8. At longer wavelengths, dual-comb spectroscopy, using two interfering laser frequency combs, has become a powerful technique capable of simultaneously providing a broad spectral range and very high resolution9. Here we demonstrate a photon-counting approach that can extend the unique advantages of this method into ultraviolet regions where nonlinear frequency conversion tends to be very inefficient. Our spectrometer, based on two frequency combs with slightly different repetition frequencies, provides a wide-span, high-resolution frequency calibration within the accuracy of an atomic clock, and overall consistency of the spectra. We demonstrate a signal-to-noise ratio at the quantum limit and an optimal use of the measurement time, provided by the multiplexed recording of all spectral data on a single photon-counter10. Our initial experiments are performed in the near-ultraviolet and in the visible spectral ranges with alkali-atom vapour, with a power per comb line as low as a femtowatt. This crucial step towards precision broadband spectroscopy at short wavelengths paves the way for extreme-ultraviolet dual-comb spectroscopy, and, more generally, opens up a new realm of applications for photon-level diagnostics, as encountered, for example, when driving single atoms or molecules.

Direct sampling of femtosecond electric-field waveforms from an optical parametric oscillator

Detecting the electric-field waveform of an optical pulse from the terahertz to the visible spectral domain provides a complete characterization of the average field waveform and holds great potential for quantum optics, time-domain (including frequency-comb) spectroscopy, high-harmonic generation, and attosecond science, to name a few. The field-resolved measurements can be performed using electro-optic sampling, where a laser pulse is characterized through an interaction with another pulse of a much shorter duration. The measured pulse train must consist of identical pulses, including their equal carrier-envelope phase (CEP). Due to the limited coverage of broadband laser gain media, creating CEP-stable pulse trains in the mid-infrared typically requires nonlinear frequency conversion, such as difference frequency generation, optical parametric amplification, or optical rectification. These techniques operate in a single-pass geometry, often limiting efficiency. In this work, we demonstrate field-resolved analysis of the pulses generated in a resonant system, an optical parametric oscillator (OPO). Due to the inherent feedback, this device exhibits a relatively high conversion efficiency at a given level of input power. By electro-optic sampling, we prove that a subharmonic OPO pumped with CEP-stable few-cycle fiber-laser pulses generates a CEP-stable mid-infrared output. The full amplitude and phase information renders dispersion control straightforward. We also confirm the existence of an exotic “flipping” state of the OPO directly in the time domain, where the electric field of consecutive pulses has the opposite sign.

Extending the propagation length of graphene plasmons via nonlinear frequency conversion

Graphene plasmons (GPs) are broadband and electrically tunable mid-infrared (MIR)/terahertz (THz) excitations, exhibiting high confinement factors exceeding two orders of magnitude. Such highly confined modes are extremely attractive for nonlinear frequency conversion owing to the large inherent field enhancement. However, this high confinement is also accompanied by losses, and together with the centrosymmetric nature of graphene practical usage of its properties in second-order nonlinear processes remains hindered. In this paper, we introduce an approach for realizing quasi-phase-matching (QPM) of propagating GPs, by placing the graphene on an orientationally patterned GaAs substrate—a transparent material in the MIR/THz range with a large second-order nonlinear coefficient. We analyze the complete frequency/Fermi-level space for QPMed second-harmonic generation of GPs in the MIR and THz and demonstrate GP amplification and loss compensation. We find that our approach provides extended GP propagation lengths that are more than twice larger than the state-of-the-art cryogenic temperature propagation lengths. The approach is general to all second-order nonlinear processes, such as sum and difference frequency generation, thus opening a path for efficient and electrically tunable QPM nonlinear processes at the atomic scale.

Robust temporal adiabatic passage with perfect frequency conversion between detuned acoustic cavities

For classical waves, phase matching is vital for enabling efficient energy transfer in many scenarios, such as waveguide coupling and nonlinear optical frequency conversion. Here, we propose a temporal quasi-phase matching method and realize robust and complete acoustical energy transfer between arbitrarily detuned cavities. In a set of three cavities, A, B, and C, the time-varying coupling is established between adjacent elements. Analogy to the concept of stimulated Raman adiabatic passage, amplitudes of the two couplings are modulated as time-delayed Gaussian functions, and the couplings’ signs are periodically flipped to eliminate temporal phase mismatching. As a result, robust and complete acoustic energy transfer from A to C is achieved. The non-reciprocal frequency conversion properties of our design are demonstrated. Our research takes a pivotal step towards expanding wave steering through time-dependent modulations and is promising to extend the frequency conversion based on state evolution in various linear Hermitian systems to nonlinear and non-Hermitian regimes.

An ultra-stable high-power optical frequency comb

Optical frequency combs are typically generated in the near-infrared wavelength range, where many mode-locked lasers operate. Nonlinear frequency conversion can then be used to extend optical frequency metrology to other spectral regions, such as the extreme ultraviolet (XUV). High-power frequency combs at the fundamental wavelength can efficiently drive nonlinear frequency conversions. Low phase noise is an important requirement because the frequency conversion process not only multiplies the carrier frequency but also the phase fluctuations. In this work, we have developed a low-noise frequency comb centered at 1030 nm with an average power of 230 W, a temporal pulse duration of 59 fs, and a peak power of 32 MW. One of the modes of the seed laser is phase-locked to a continuous wave reference laser stabilized to an ultra-stable high-finesse cavity. The residual integrated phase noise from 10 Hz to 10 MHz is 41 mrad, which is sufficiently low to address narrow transitions with kHz-level linewidths after the frequency conversion to XUV wavelengths.