Showing papers on "Four-wave mixing published in 2016"

Plasmonic nanofocused four-wave mixing for femtosecond near-field imaging

Abstract: Femtosecond nonlinear optical imaging with nanoscale spatial resolution would provide access to coupled degrees of freedom and ultrafast response functions on the characteristic length scales of electronic and vibrational excitations. Although near-field microscopy provides the desired spatial resolution, the design of a broadband high-contrast nanoprobe for ultrafast temporal resolution is challenging due to the inherently weak nonlinear optical signals generated in subwavelength volumes. Here, we demonstrate broadband four-wave mixing with enhanced nonlinear frequency conversion efficiency at the apex of a nanometre conical tip. Far-field light is coupled through a grating at the shaft of the tip, generating plasmons that propagate to the apex while undergoing asymptotic compression and amplification, resulting in a nonlinear conversion efficiency of up to 1 × 10(-5). We apply this nonlinear nanoprobe to image the few-femtosecond coherent dynamics of plasmonic hotspots on a nanostructured gold surface with spatial resolution of a few tens of nanometres. The approach can be generalized towards spatiotemporal imaging and control of coherent dynamics on the nanoscale, including the extension to multidimensional spectroscopy and imaging.

Radiatively Limited Dephasing and Exciton Dynamics in MoSe2 Monolayers Revealed with Four-Wave Mixing Microscopy.

Abstract: By implementing four-wave mixing (FWM) microspectroscopy, we measure coherence and population dynamics of the exciton transitions in monolayers of MoSe2. We reveal their dephasing times T2 and radiative lifetime T1 in a subpicosecond (ps) range, approaching T2 = 2T1 and thus indicating radiatively limited dephasing at a temperature of 6 K. We elucidate the dephasing mechanisms by varying the temperature and by probing various locations on the flake exhibiting a different local disorder. At the nanosecond range, we observe the residual FWM produced by the incoherent excitons, which initially disperse toward the dark states but then relax back to the optically active states within the light cone. By introducing polarization-resolved excitation, we infer intervalley exciton dynamics, revealing an initial polarization degree of around 30%, constant during the initial subpicosecond decay, followed by the depolarization on a picosecond time scale. The FWM hyperspectral imaging reveals the doped and undoped area...

Low-noise kinetic inductance traveling-wave amplifier using three-wave mixing

Abstract: We have fabricated a wide-bandwidth, high dynamic range, low-noise cryogenic amplifier based on a superconducting kinetic inductance traveling-wave device. The device was made from NbTiN and consisted of a long, coplanar waveguide on a silicon chip. By adding a DC current and an RF pump tone, we are able to generate parametric amplification using three-wave mixing (3WM). The devices exhibit gain of more than 15 dB across an instantaneous bandwidth from 4 to 8 GHz. The total usable gain bandwidth, including both sides of the signal-idler gain region, is more than 6 GHz. The noise referred to the input of the devices approaches the quantum limit, with less than 1 photon excess noise. We compare these results directly to the four-wave mixing amplification mode, i.e., without DC-biasing. We find that the 3WM mode allows operation with the pump at lower RF power and at frequencies far from the signal. We have used this knowledge to redesign the amplifiers to utilize primarily 3WM amplification, thereby allowing for direct integration into large scale qubit and detector applications.

Few-photon coherent nonlinear optics with a single molecule

Abstract: Photons are efficiently funnelled into a single molecule if they are nearly resonant with the sharp molecular transition. In this condition, the coherent nonlinear optical effect can be induced with only a few photons without high-finesse cavities.

Quantum dynamics of Kerr optical frequency combs below and above threshold: Spontaneous four-wave mixing, entanglement, and squeezed states of light

Abstract: The dynamical behavior of Kerr optical frequency combs is very well understood today from the perspective of the semiclassical approximation. These combs are obtained by pumping an ultrahigh-$Q$ whispering-gallery mode resonator with a continuous-wave laser. The long-lifetime photons are trapped within the toruslike eigenmodes of the resonator, where they interact nonlinearly via the Kerr effect. In this article, we use quantum Langevin equations to provide a theoretical understanding of the nonclassical behavior of these combs when pumped below and above threshold. In the configuration where the system is under threshold, the pump field is the unique oscillating mode inside the resonator, and it triggers the phenomenon of spontaneous four-wave mixing, where two photons from the pump are symmetrically up- and down-converted in the Fourier domain. This phenomenon, also referred to as parametric fluorescence, can only be understood and analyzed from a fully quantum perspective as a consequence of the coupling between the field of the central (pumped) mode and the vacuum fluctuations of the various side modes. We analytically calculate the power spectra of the spontaneous emission noise, and we show that these spectra can be either single- or double-peaked depending on the value of the laser frequency, chromatic dispersion, pump power, and spectral distance between the central mode and the side mode of interest. We also calculate as well the overall spontaneous noise power per side mode and propose simplified analytical expressions for some particular cases. In the configuration where the system is pumped above threshold, we investigate the phenomena of quantum correlations and multimode squeezed states of light that can occur in the Kerr frequency combs originating from stimulated four-wave mixing. We show that for all stationary spatiotemporal patterns, the side modes that are symmetrical relative to the pumped mode in the frequency domain display quantum correlations that can lead to squeezed states of light under some optimal conditions that are analytically determined. These quantum correlations can persist regardless the dynamical state of the system (rolls or solitons), regardless of the spectral extension of the comb (number side modes) and regardless of the dispersion regime (normal or anomalous). We also explicitly determine the phase quadratures leading to photon entanglement and analytically calculate their quantum-noise spectra. For both the below- and above-threshold cases, we study with particular emphasis the two principal architectures for Kerr comb generation, namely the add-through and add-drop configurations. It is found that regardless of the configuration, an essential parameter is the ratio between out-coupling and total losses, which plays a key role as it directly determines the efficiency of the detected fluorescence or squeezing spectra. We finally discuss the relevance of Kerr combs for quantum information systems at optical telecommunication wavelengths below and above threshold.

Phase matching for spontaneous frequency conversion via four-wave mixing in graded-index multimode optical fibers

Abstract: A detailed analysis of four-wave mixing (FWM) and its required phase-matching conditions in graded-index multimode optical fibers is presented. The analysis is relevant mainly for spontaneous frequency conversion and photon pair generation via FWM, when the fiber length is of the order of a meter or shorter, and the signal and idler are generated at large frequency separations from the pump. An analytic expression for calculating the phase mismatch occurring as a result of the waveguide dispersion among the pump, signal, and idler beams is derived, and it agrees well with independent numerical analysis. This expression simplifies calculations considerably, as it allows the prediction of the wavelengths of the signal and idler by using only the mode group number of the spatial modes involved in the FWM process and the refractive index profile of the fiber. The scaling of the signal–pump–idler frequency separations with the mode group numbers is explored. The abundance of the configuration degeneracies of the FWM process in graded-index multimode fibers indicates that nearly identical signal and idler frequencies can be obtained for many different pump, signal, and idler spatial mode profile combinations.

Four-wave mixing parametric oscillation and frequency comb generation at visible wavelengths in a silica microbubble resonator.

Abstract: Frequency comb generation in microresonators at visible wavelengths has found applications in a variety of areas such as metrology, sensing, and imaging. To achieve Kerr combs based on four-wave mixing in a microresonator, dispersion must be in the anomalous regime. In this Letter, we demonstrate dispersion engineering in a microbubble resonator (MBR) fabricated by a two-CO2 laser beam technique. By decreasing the wall thickness of the MBR to 1.4 μm, the zero dispersion wavelength shifts to values shorter than 764 nm, making phase matching possible around 765 nm. With the optical Q-factor of the MBR modes being greater than 107, four-wave mixing is observed at 765 nm for a pump power of 3 mW. By increasing the pump power, parametric oscillation is achieved, and a frequency comb with 14 comb lines is generated at visible wavelengths.

Inter-modal four-wave mixing study in a two-mode fiber

Abstract: We demonstrate efficient four-wave mixing among different spatial modes in a 1-km long two-mode fiber at telecommunication wavelengths. Two pumps excite the LP01 and LP11 modes, respectively, while the probe signal excites the LP01 mode, and the phase conjugation (PC) and Bragg scattering (BS) idlers are generated in the LP11 mode. For these processes we experimentally characterize their phase matching efficiency and bandwidth and find that they depend critically on the wavelength separation of the two pumps, in good agreement with the numerical study we carried out. We also confirm experimentally that BS has a larger bandwidth than PC for the optimum choice of the pump wavelength separation.

Time domain modeling of terahertz quantum cascade lasers for frequency comb generation.

Abstract: The generation of frequency combs in the mid-infrared and terahertz regimes from compact and potentially cheap sources could have a strong impact on spectroscopy, as many molecules have their rotovibrational bands in this spectral range. Thus, quantum cascade lasers (QCLs) are the perfect candidates for comb generation in these portions of the electromagnetic spectrum. Here we present a theoretical model based on a full numerical solution of Maxwell-Bloch equations suitable for the simulation of such devices. We show that our approach captures the intricate interplay between four wave mixing, spatial hole burning, coherent tunneling and chromatic dispersion which are present in free running QCLs. We investigate the premises for the generation of QCL based terahertz combs. The simulated comb spectrum is in good agreement with experiment, and also the observed temporal pulse switching between high and low frequency components is reproduced. Furthermore, non-comb operation resulting in a complex multimode dynamics is investigated.

On Frequency Combs in Monolithic Resonators

Abstract: Abstract Optical frequency combs have become indispensable in astronomical measurements, biological fingerprinting, optical metrology, and radio frequency photonic signal generation. Recently demonstrated microring resonator-based Kerr frequency combs point the way towards chip scale optical frequency comb generator retaining major properties of the lab scale devices. This technique is promising for integrated miniature radiofrequency and microwave sources, atomic clocks, optical references and femtosecond pulse generators. Here we present Kerr frequency comb development in a historical perspective emphasizing its similarities and differences with other physical phenomena. We elucidate fundamental principles and describe practical implementations of Kerr comb oscillators, highlighting associated solved and unsolved problems.

Energy correlations of photon pairs generated by a silicon microring resonator probed by Stimulated Four Wave Mixing

Abstract: Compact silicon integrated devices, such as micro-ring resonators, have recently been demonstrated as efficient sources of quantum correlated photon pairs. The mass production of integrated devices demands the implementation of fast and reliable techniques to monitor the device performances. In the case of time-energy correlations, this is particularly challenging, as it requires high spectral resolution that is not currently achievable in coincidence measurements. Here we reconstruct the joint spectral density of photons pairs generated by spontaneous four-wave mixing in a silicon ring resonator by studying the corresponding stimulated process, namely stimulated four wave mixing. We show that this approach, featuring high spectral resolution and short measurement times, allows one to discriminate between nearly-uncorrelated and highly-correlated photon pairs.

Coherent mid-infrared frequency combs in silicon-microresonators in the presence of Raman effects

Abstract: We demonstrate the first low-noise mid-IR frequency comb source using a silicon microresonator. Our observation of strong Raman scattering lines in the generated comb suggests that interplay between Raman and four-wave mixing plays a role in the generated low-noise state. In addition, we characterize, the intracavity comb generation dynamics using an integrated PIN diode, which takes advantage of the inherent three-photon absorption process in silicon.

Four-wave mixing parametric oscillation and frequency comb generation at visible wavelengths in a silica microbubble resonator

Abstract: Frequency comb generation in microresonators at visible wavelengths has found applications in a variety of areas such as metrology, sensing, and imaging. To achieve Kerr combs based on four-wave mixing in a microresonator, dispersion must be in the anomalous regime. In this work, we demonstrate dispersion engineering in a microbubble resonator (MBR) fabricated by a two-CO$_2$ laser beam technique. By decreasing the wall thickness of the MBR down to 1.4 $\mu$m, the zero dispersion wavelength shifts to values shorter than 764 nm, making phase matching possible around 765 nm. With the optical \textit{Q}-factor of the MBR modes being greater than $10^7$, four-wave mixing is observed at 765 nm for a pump power of 3 mW. By increasing the pump power, parametric oscillation is achieved, and a frequency comb with 14 comb lines is generated at visible wavelengths.

Fiber-based photon-pair source capable of hybrid entanglement in frequency and transverse mode, controllably scalable to higher dimensions

Abstract: We have designed and implemented a photon-pair source, based on the spontaneous four wave mixing (SFWM) process in a few-mode fiber, in a geometry which permits multiple, simultaneous SFWM processes, each associated with a distinct combination of transverse modes for the four participating waves. In our source: i) each process is group-velocity-matched so that it is, by design, nearly-factorable and ii) the spectral separation between neighboring processes is greater than the marginal spectral width of each process. Consequently, there is a direct correspondence between the joint amplitude of each process and each of the Schmidt mode pairs of the overall two-photon state. Our approach permits hybrid entanglement in discrete frequency and in transverse mode, whereby control of the number of supported fiber transverse modes allows scalability to higher dimensions while spectral filtering may be used for straightforward Schmidt mode discrimination.

Time-resolved four-wave-mixing spectroscopy for inner-valence transitions

Abstract: Noncollinear four-wave-mixing (FWM) techniques at near-infrared (NIR), visible, and ultraviolet frequencies have been widely used to map vibrational and electronic couplings, typically in complex molecules. However, correlations between spatially localized inner-valence transitions among different sites of a molecule in the extreme ultraviolet (XUV) spectral range have not been observed yet. As an experimental step toward this goal, we perform time-resolved FWM spectroscopy with femtosecond NIR and attosecond XUV pulses. The first two pulses (XUV-NIR) coincide in time and act as coherent excitation fields, while the third pulse (NIR) acts as a probe. As a first application, we show how coupling dynamics between odd- and even-parity, inner-valence excited states of neon can be revealed using a two-dimensional spectral representation. Experimentally obtained results are found to be in good agreement with ab initio time-dependent R-matrix calculations providing the full description of multielectron interactions, as well as few-level model simulations. Future applications of this method also include site-specific probing of electronic processes in molecules.

Enhancement of four-wave mixing via interference of multiple plasmonic conversion paths

Abstract: Recent experiments demonstrate that plasmonic resonators can enhance the four-wave mixing (FWM) process by several orders of magnitude, due to the localization of the incident fields. We show that, when the plasmonic resonator is coupled to two quantum emitters, a three orders of magnitude enhancement can be obtained on top of the enhancement due to the localization. We explicitly demonstrate---on an expression for the steady-state FWM amplitude---how the presence of a Fano resonance leads to the cancellation of nonresonant terms in a FWM process. A cancellation in the denominator gives rise to an enhancement in the nonlinearity. The explicit demonstration we present here guides one to a method for achieving even larger enhancement factors by introducing additional coupling terms. The method is also applicable to Fano resonances induced by all-plasmonic couplings, which are easier to control in experiments.

Near-resonant four-wave mixing of attosecond extreme-ultraviolet pulses with near-infrared pulses in neon: Detection of electronic coherences

Abstract: Coherent narrow-band extreme-ultraviolet (EUV) light is generated by a near-resonant four-wave mixing (FWM) process between attosecond pulse trains and near-infrared pulses in neon gas. The near-resonant FWM process involves one vacuum-ultraviolet (VUV) photon and two near-infrared (NIR) photons and produces new higher-energy frequency components corresponding to the $ns/nd$ to ground-state $(2{s}^{2}2{p}^{6})$ transitions in the neon atom. The EUV emission exhibits small angular divergence (2 mrad) and monotonically increasing intensity over a pressure range of 0.5--16 Torr, suggesting phase matching in the production of the narrow-bandwidth coherent EUV light. In addition, time-resolved scans of the NIR nonlinear mixing process reveal the detection of a persistent, ultrafast bound electronic wave packet based on a coherent superposition initiated by the VUV pulse in the neon atoms. This FWM process using attosecond pulses offers a means for both efficient narrow-band EUV source generation and time-resolved investigations of ultrafast dynamics.

Simultaneous observation of free and defect-bound excitons in CH 3 NH 3 PbI 3 using four-wave mixing spectroscopy

Abstract: Solar cells incorporating organic-inorganic perovskite, which may be fabricated using low-cost solution-based processing, have witnessed a dramatic rise in efficiencies yet their fundamental photophysical properties are not well understood. The exciton binding energy, central to the charge collection process, has been the subject of considerable controversy due to subtleties in extracting it from conventional linear spectroscopy techniques due to strong broadening tied to disorder. Here we report the simultaneous observation of free and defect-bound excitons in CH3NH3PbI3 films using four-wave mixing (FWM) spectroscopy. Due to the high sensitivity of FWM to excitons, tied to their longer coherence decay times than unbound electron- hole pairs, we show that the exciton resonance energies can be directly observed from the nonlinear optical spectra. Our results indicate low-temperature binding energies of 13 meV (29 meV) for the free (defect-bound) exciton, with the 16 meV localization energy for excitons attributed to binding to point defects. Our findings shed light on the wide range of binding energies (2-55 meV) reported in recent years.

Determination of the electric field strength of filamentary DBDs by CARS-based four-wave mixing

Abstract: It is demonstrated that a four-wave mixing technique based on coherent anti-Stokes Raman spectroscopy (CARS) can determine the electric field strength of a pulsed-driven filamentary dielectric barrier discharge (DBD) of 1 mm gap, using hydrogen as a tracer medium in nitrogen at atmospheric pressure. The measurements are presented for a hydrogen admixture of 10%, but even 5% H2 admixture delivers sufficient infrared signals. The lasers do not affect the discharge by photoionization or by other radiation-induced processes. The absolute values of the electric field strength can be determined by the calibration of the CARS setup with high voltage amplitudes below the ignition threshold of the arrangement. This procedure also enables the determination of the applied breakdown voltage. The alteration of the electric field is observed during the internal polarity reversal and the breakdown process. One advantage of the CARS technique over emission-based methods is that it can be used independently of emission, e.g. in the pre-phase and in between two consecutive discharges, where no emission occurs at all.

Measurements of the nonlinear refractive index of air, N 2 , and O 2 at 10 μm using four-wave mixing.

Abstract: We report on measurements of the nonlinear index of refraction of air, N2, and O2 at a wavelength close to 10 μm by collinear four-wave mixing of a 200 MW CO2 laser beat-wave. The use of a 200 ps long beat-wave comprising radiation amplified on the 10P20 and 10R16 lines of the CO2 laser provides a sensitive method to measure the small nonlinearities characteristic of the gas phase in a spectral region where no such data exists.

Stimulated Brillouin scattering and Brillouin-coupled four-wave-mixing in a silica microbottle resonator.

Abstract: We report the first observation of stimulated Brillouin scattering (SBS) with Brillouin lasing, and Brillouin-coupled four-wave-mixing (FWM) in an ultra-high-Q silica microbottle resonator. The Brillouin lasing was observed at the frequency of ΩB = 2π × 10.4 GHz with a threshold power of 0.45 mW. Coupling between Brillouin and FWM was observed in both backward and forward scattering directions with separations of 2ΩB. At a pump power of 10 mW, FWM spacing reached to 7th and 9th order anti-Stokes and Stokes, respectively.

Correlated photon pair generation in AlGaAs nanowaveguides via spontaneous four-wave mixing.

Abstract: We demonstrate a source of correlated photon pairs which will have applications in future integrated quantum photonic circuits. The source utilizes spontaneous four-wave mixing (SFWM) in a dispersion-engineered nanowaveguide made of AlGaAs, which has merits of negligible two-photon absorption and low spontaneous Raman scattering (SpRS). We observe a coincidence-to-accidental (CAR) ratio up to 177, mainly limited by propagation losses. Experimental results agree well with theoretical predictions of the SFWM photon pair generation and the SpRS noise photon generation. We also study the effects from the SpRS, propagation losses, and waveguide lengths on the quality of our source.

Photon pair generation by intermodal spontaneous four wave mixing in birefringent, weakly guiding optical fibers

Abstract: We present a theoretical and experimental study of the generation of photon pairs through the process of spontaneous four-wave mixing (SFWM) in a few-mode, birefringent fiber. Under these conditions, multiple SFWM processes are in fact possible, each associated with a different combination of transverse modes for the four waves involved. We show that in the weakly guiding regime, for which the propagation modes may be well approximated by linearly polarized modes, the departure from circular symmetry due to the fiber birefringence translates into conservation rules, which retain elements from azimuthal and rectangular symmetries: both OAM and parity must be conserved for a process to be viable. We have implemented a SFWM source based on a bowtie birefringent fiber, and have measured for a collection of pump wavelengths the SFWM spectra of each of the signal and idler photons in coincidence with its partner photon. We have used this information, together with knowledge of the transverse modes into which the signal and idler photons are emitted, as input for a genetic algorithm, which accomplishes two tasks: (i) the identification of the particular SFWM processes that are present in the source, and (ii) the characterization of the fiber used.

Stimulated Brillouin scattering and Brillouin-coupled four-wave-mixing in a silica microbottle resonator

Abstract: We report the first observation of stimulated Brillouin scattering (SBS) with Brillouin lasing, and Brillouin-coupled four-wave-mixing (FWM) in an ultra-high-Q silica microbottle resonator. The Brillouin lasing was observed at the frequency of $\Omega_B=2\pi\times10.4$ GHz with a threshold power of $0.45$ mW. Coupling between Brillouin and FWM was observed in both backward and forward scattering directions with separations of $2\Omega_B$. At a pump power of $10$ mW, FWM spacing reached to 7th and 9th order anti-Stokes and Stokes, respectively.

Degenerate four-wave mixing in silicon hybrid plasmonic waveguides.

Abstract: Silicon-based plasmonic waveguides show high confinement well beyond the diffraction limit. Various devices have been demonstrated to outperform their dielectric counterparts at micrometer scales, such as linear modulators, capable of generating high field confinement and improving device efficiency by increasing access to nonlinear processes, limited by ohmic losses. By using hybridized plasmonic waveguide architectures and nonlinear materials, silicon-based plasmonic waveguides can generate strong nonlinear effects over just a few wavelengths. We have theoretically investigated the nonlinear optical performance of two hybrid plasmonic waveguides (HPWG) with three different nonlinear materials. Based on this analysis, the hybrid gap plasmon waveguide (HGPW), combined with the DDMEBT nonlinear polymer, shows a four-wave mixing (FWM) conversion efficiency of -16.4 dB over a 1 μm propagation length, demonstrating that plasmonic waveguides can be competitive with standard silicon photonics structures over distances three orders of magnitude shorter.

High-speed all-optical NAND/AND logic gates using four-wave mixing Bragg scattering

Abstract: A high-speed all-optical NAND logic gate is proposed and experimentally demonstrated using four-wave mixing Bragg scattering in highly nonlinear fiber. NAND/AND logic functions are implemented at two wavelengths by encoding logic inputs on two pumps via on–off keying. A 15.2-dB depletion of the signal is obtained for NAND operation, and time domain measurements show 10-Gb/s NAND/AND logic operations with open eye diagrams. The approach can be readily extended to higher data rates and transferred to on-chip waveguide platforms.

Enhanced four-wave mixing with nonlinear plasmonic metasurfaces

Abstract: Plasmonic metasurfaces provide an effective way to increase the efficiency of several nonlinear processes while maintaining nanoscale dimensions. In this work, nonlinear metasurfaces based on film-coupled silver nanostripes loaded with Kerr nonlinear material are proposed to achieve efficient four-wave mixing (FWM). Highly localized plasmon resonances are formed in the nanogap between the metallic film and nanostripes. The local electric field is dramatically enhanced in this subwavelength nanoregion. These properties combined with the relaxed phase matching condition due to the ultrathin area lead to a giant FWM efficiency, which is enhanced by nineteen orders of magnitude compared to a bare silver screen. In addition, efficient visible and low-THz sources can be constructed based on the proposed nonlinear metasurfaces. The FWM generated coherent wave has a directional radiation pattern and its output power is relatively insensitive to the incident angles of the excitation sources. This radiated power can be further enhanced by increasing the excitation power. The dielectric nonlinear material placed in the nanogap is mainly responsible for the ultrastrong FWM response. Compact and efficient wave mixers and optical sources spanning different frequency ranges are envisioned to be designed based on the proposed nonlinear metasurface designs.

Broad bandwidth third-harmonic generation via four-wave mixing and stimulated Raman scattering in a microcavity.

Abstract: We generate broad bandwidth visible light ranging from 498 to 611 nm via third-harmonic generation in a silica toroid microcavity. The silica toroid microcavity is fed with a continuous-wave input at a telecom wavelength, where third-harmonic generation follows the generation of an infrared Kerr comb via cascaded four-wave-mixing and stimulated Raman scattering effects. Thanks to these cascaded effects (four-wave mixing, stimulated Raman scattering, and third-harmonic generation) in an ultrahigh-Q microcavity, a broad bandwidth visible light is obtained. The visible light couples with the whispering gallery mode of the cavity by demonstrating the evanescent coupling of the generated visible light with a tapered fiber based on an add-drop configuration.

Enhanced four-wave mixing with nonlinear plasmonic metasurfaces

Abstract: Plasmonic metasurfaces provide an effective way to increase the efficiency of several nonlinear processes while maintaining nanoscale dimensions. In this work, nonlinear metasurfaces based on film-coupled silver nanostripes loaded with Kerr nonlinear material are proposed to achieve efficient four-wave mixing (FWM). Highly localized plasmon resonances are formed in the nanogap between the metallic film and nanostripes. The local electric field is dramatically enhanced in this subwavelength nanoregion. These properties combined with the relaxed phase matching condition due to the ultrathin area lead to a giant FWM efficiency, which is enhanced by nineteen orders of magnitude compared to a bare silver screen. In addition, efficient visible and low-THz sources can be constructed based on the proposed nonlinear metasurfaces. The FWM generated coherent wave has a directional radiation pattern and its output power is relatively insensitive to the incident angles of the excitation sources. This radiated power can be further enhanced by increasing the excitation power. The dielectric nonlinear material placed in the nanogap is mainly responsible for the ultrastrong FWM response. Compact and efficient wave mixers and optical sources spanning different frequency ranges are envisioned to be designed based on the proposed nonlinear metasurface designs.

Dynamics of excitons in individual InAs quantum dots revealed in four-wave mixing spectroscopy

Abstract: A detailed understanding of the population and coherence dynamics in optically driven individual emitters in solids and their signatures in ultrafast nonlinear-optical signals is of prime importance for their applications in future quantum and optical technologies. In a combined experimental and theoretical study on exciton complexes in single semiconductor quantum dots we reveal a detailed picture of the dynamics employing three-beam polarization-resolved four-wave mixing (FWM) micro-spectroscopy. The oscillatory dynamics of the FWM signals in the exciton-biexciton system is governed by the fine-structure splitting and the biexciton binding energy in an excellent quantitative agreement between measurement and analytical description. The analysis of the excitation conditions exhibits a dependence of the dynamics on the specific choice of polarization configuration, pulse areas and temporal ordering of driving fields. The interplay between the transitions in the four-level exciton system leads to rich evolution of coherence and population. Using two-dimensional FWM spectroscopy we elucidate the exciton-biexciton coupling and identify neutral and charged exciton complexes in a single quantum dot. Our investigations thus clearly reveal that FWM spectroscopy is a powerful tool to characterize spectral and dynamical properties of single quantum structures.