Third Harmonic Generation Research Articles

Maximum chirality of THz metasurfaces with quasi-bound states in the continuum.

Metasurfaces hold great promise for terahertz (THz) chiral-optical devices. Here, we proposed a chiral THz metasurface with quasi-bound state in the continuum (BIC) for maximum chirality. By exploiting structural perturbations of the dipole displacement and the diverging angle for the THz metasurface, the symmetry-protected BIC transforms into quasi-BIC. The critical coupling condition is satisfied by the introduction of graphene, enabling the theoretical maximum absorption of the quasi-BIC. Subsequently, the perturbations are balanced to obtain maximum chirality. The numerical simulations show that the THz metasurface exhibits strong linear chirality with the circular dichroism (CD) of 0.99 at the quasi-BIC. Additionally, the chiral third harmonic generation (THG) is achieved, characterized by high efficiency up to 19% and strong THG-CD as high as 0.99. It is expected that the THz metasurfaces has great potential for applications in chiral sensing and imaging.

Third Harmonic Generation in Thin NbOI2 and TaOI2.

The niobium oxide dihalides have recently been identified as a new class of van der Waals materials exhibiting exceptionally large second-order nonlinear optical responses and robust in-plane ferroelectricity. In contrast to second-order nonlinear processes, third-order optical nonlinearities can arise irrespective of whether a crystal lattice is centrosymmetric. Here, we report third harmonic generation (THG) in two-dimensional (2D) transition metal oxide iodides, namely NbOI2 and TaOI2. We observe a comparable THG intensity from both materials. By benchmarking against THG from monolayer WS2, we deduce that the third-order susceptibility is approximately on the same order. THG resonances are revealed at different excitation wavelengths, likely due to enhancement by excitonic states and band edge resonances. The THG intensity increases for material thicknesses up to 30 nm, owing to weak interlayer coupling. After this threshold, it shows saturation or a decrease, due to optical interference effects. Our results establish niobium and tantalum oxide iodides as promising 2D materials for third-order nonlinear optics, with intrinsic in-plane ferroelectricity and thickness-tunable nonlinear efficiency.

Realizing high-efficiency third harmonic generation via accidental bound states in the continuum.

The bound states in the continuum (BICs) have attracted much attention in designing metasurface due to their high Q-factor and effectiveness in suppressing radiational loss. Here we report on the realization of the third harmonic generation (THG) at a near-ultraviolet wavelength (343 nm) via accidental BICs in a metasurface. The absolute conversion efficiency of the THG reaches 1.13 × 10-5 at a lower peak pump intensity of 0.7 GW/cm2. This approach allows the generation of an unprecedentedly high nonlinear conversion efficiency with simple structures.

Enhanced terahertz frequency mixing in all-dielectric metamaterial with multiple surface plasmon polaritons resonances

Nonlinear metamaterials hold a promising platform for generating terahertz (THz) waves. In this paper, we present an all-dielectric metamaterial with multiple surface plasmon polariton (SPP) resonances for enhanced THz frequency mixing. The metamaterial is composed of graphene ribbons, a dielectric layer, and a one-dimensional photonic crystal, displaying the multiple absorptions with simultaneous excitation of three SPP resonances. Taking advantage of SPP resonances with high Q factor and strong localized field at the input frequency, the third-order nonlinear processes are remarkably enhanced, including third-harmonic generation and four-wave mixing, producing a variety of frequencies in the THz range. The proposed efficient nonlinear metamaterials offer promising applications for THz frequency synthesis.

Third harmonic generation due to free carrier in InSb using a terahertz free electron laser.

We report on the third harmonic generation (THG) in InSb semiconductor irradiated by a terahertz (THz) free electron laser (FEL). The conversion of 4 THz (wavelength 70 µm) FEL outputs into its third harmonic 12 THz was observed. We found that by tuning the sample temperature to 360 K, high conversion efficiency up to 1% can be obtained and is the highest in the THz and FIR regions below 10 THz. We also discuss the observed intensity dependence of the THG with the nonlinear order lower than 3 when the pumping intensity was high.

Dynamical interplay between superconductivity and pseudogap in cuprates as revealed by terahertz third-harmonic generation spectroscopy

We report on nonlinear terahertz third-harmonic generation (THG) measurements on YBa 2 Cu 3 O 6+ x thin films. Different from conventional superconductors, the THG signal starts to appear in the normal state, which is consistent with the crossover temperature T * of pseudogap over broad doping levels. Upon lowering the temperature, the THG signal shows an anomaly just below T c in the optimally doped sample. Notably, we observe a beat pattern directly in the measured real-time waveform of the THG signal. We elaborate that the Higgs mode, which develops below T c , couples to the mode already developed below T * , resulting in an energy level splitting. However, this coupling effect is not evident in underdoped samples. We explore different potential explanations for the observed phenomena. Our research offers valuable insight into the interplay between superconductivity and pseudogap.

Efficient Third Harmonic Generation from Magnetic Resonance in Low-Index Dielectric Nanopillars

Boosting the harmonic generation of light in nanostructures through efficiently enhancing the light–matter interaction has received enormous attention and applications. Low-index dielectric nanoparticles, as one of the crucial members of nanophotonics, have not been successful in nonlinear enhancement due to weak Mie resonance and poor light confinement. Here, we designed efficient third harmonic generation (THG) in low-index dielectric nanopillars sandwiched by double layers of metal dressing (Au/polymer/Au), where the polymer offers essential nonlinear susceptibility. The resonance of the low-index nanopillars significantly enhanced the scattering and had a strong magnetic response that could boost the THG effect. We predict that the THG efficiency reaches up to 3 × 10−6 (six orders of enhancement) at a third harmonic wavelength of 300 nm. The efficient THG in low-index dielectric nanopillars may open the possibility for the development of a new type of efficient nonlinear coherent source.

Giant enhancement of third harmonic generation in an array of graphene ribbons using amplification of surface plasmon polaritons by optical gain

In this paper, we theoretically study the enhancement of third-harmonic generation in a plasmonic structure composed of an array of trilayer graphene ribbons sandwiched between two CaF2\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$CaF_{2}$$\\end{document} layers. In fact, we suggest a new method for more enhancement of nonlinearity in plasmonic structures using incorporation of optical gain into graphene ribbons. As the pump intensity increases, the maximum output intensity of third harmonic generated (THG) wave versus fundamental frequency is blue-shifted while its value enhances. Our analysis indicates that the enhancement factor of THG in our proposed structure is 1.1 × 107 without occurring an electric breakdown compared to case at which an optically pumped trilayer graphene sheet sandwiched between two CaF2 layers. Therefore, only presence of optical gain is not sufficient for significant enhancement of output intensity of THG wave and excitation of SPPs through the structure is also essential. On the other hand, our results demonstrate that the output intensity of THG wave from the proposed structure under optical pumping enhances by 105\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$10^{5}$$\\end{document} times compared to the plasmonic structure without optical gain which confirms the role of optical gain for THG enhancement in the plasmonic structure. This is because the gain in graphene ribbons amplifies the SPPs waves leading to the more field enhancement along the graphene ribbons which results in significant enhancement of THG wave in the plasmonic structure in comparison with one without gain. Therefore, we reveal that both SPPs and optical gain contribute to the strong output intensity of THG in our proposed structure compared to the trilayer graphene sheet inserted between two CaF2 layers.

Polarization-insensitive and polarization-controlled dual-band third-harmonic generation in silicon metasurfaces driven by quasi-bound states in the continuum

High-refractive-index nanostructures offer versatile opportunities for nonlinear optical effects, due to their ability to strongly confine field into a subwavelength scale. Herein, we propose a rhomboidal amorphous silicon metasurface to realize high-efficiency dual-band third-harmonic generation (THG), based on the supported dual quasi-bound states in the continuum (Q-BICs). Owing to the very large field confinement inside the metasurface empowered by Q-BICs, the THG efficiency up to 3.74 × 10−3 with the peak pump intensity of 30 MW/cm2 is observed. Meanwhile, thanks to the very high quality factor of Q-BICs, the ultra-narrow nonlinear process with the full width at half maximum less than 1 nm is also witnessed, suggesting the good monochromaticity. Interestingly, the dual-band THG is verified to be polarization-dependent and polarization-insensitive, respectively. The finite element method simulations exhibit that the polarization-dependent THG is attributed to the Q-BIC driven by the electric quadrupole characterized by a pair of anti-parallel electric dipoles along the x axis, which are only excited by the x-linearly polarized light. On the contrary, the polarization-insensitive THG is enabled by another Q-BIC governed by the magnetic dipole resonance with circular electric field vectors, which can be excited by any linearly polarized light. The polarization-controlled and polarization-independent dual-band THG enabled by the physics of Q-BICs would open possibilities for designing switchable nonlinear light sources. The proposed dual Q-BICs scheme undoubtedly can serve as a universal recipe for other nonlinear effects, including sum-frequency generation, difference-frequency generation, and high-order harmonics.

Generation of 351 nm UV Q-switched laser beam with controllable spatial coherence

Ultraviolet laser with controllable spatial coherence is essential for a wide range of applications. In this study, we developed a pulsed, partially spatial coherence laser source operating in the ultraviolet (UV) range through extra-cavity frequency tripling of a solid-state Nd:glass degenerate laser. The oscillating modes of the laser can be flexibly controlled by size of the spatial filter inside the laser cavity, thus modulating the spatial coherence of the UV laser. The beam pattern and focusing, speckle suppression and imaging, coherence property of the partially coherent UV laser is investigated in detail. The third-harmonic generation (THG) supports many more transverse modes than the fundamental generation and the second-harmonic generation (SHG). Compared with high coherent UV laser, low spatial coherent UV laser has better speckle suppression effect and smoother focused spot intensity distribution. The high brightness, good monochromaticity and low spatial coherence make the UV degenerate laser an attractive illumination source for inertial confinement fusion, lithography, laser processing and others.

Enhanced optical third-harmonic generation in phase-engineered nanostructured Zn1−x Cd x S thin films for optoelectronic device applications

A polycrystalline nanostructured thin film of zinc cadmium sulfide was meticulously fabricated on a glass substrate using the thermal evaporation method physical vapor deposition within a vacuum chamber. Different doping concentrations were introduced by varying the cadmium (Cd) content, resulting in Zn1-x Cd x S films with Cd concentrations ranging from x = 0.00–0.20 wt %. The impact of Cd doping on the third-order nonlinear optical (TONLO) properties of these films was thoroughly studied using the Z-scan method, employing a diode-pumped solid-state continuous-wave laser. To gain insight into the structural characteristics, the Zn1-x Cd x S thin films underwent analysis through x-ray diffraction. Optical studies confirmed the tunability of the optical band gap (Eg) in the Zn1-x Cd x S films, ranging from 3.88 eV for undoped ZnS to 2.80 eV for the film fabricated with 20 wt. % of Cd-content. This significant reduction in ‘Eg’ renders the films highly suitable for use as absorbing layers in applications such as solar cells and optoelectronics. Surface morphology analysis, performed via field emission scanning electron microscopy, revealed noticeable alterations with increased Cd doping. Significantly, the doped films exhibited a substantial redshift in the band edge and an increase in transmittance within the visible and near-infrared regions. The investigation of TONLO properties, including the nonlinear absorption coefficient (β), nonlinear refractive index (n 2) and susceptibility χ(3), yielded values ranging from 3.15 × 10−3 to 8.16 × 10−3 (cm W−1), 1.65 × 10−8 to 7.45 x 10–8 (cm2 W−1), and 3.12 × 10−5 to 7.86 × 10−5 (esu), respectively. These results indicate the presence of self-defocusing nonlinearity in the films. Overall, the outcomes underscore the potential of Cd-doped ZnS nanostructures in modifying surface morphology and enhancing NLO characteristics. Zn1-x Cd x S thin films exhibit promise for applications in nonlinear optical devices, as evidenced by these encouraging findings.

Modal Phase-Matched Bound States in the Continuum for Enhancing Third Harmonic Generation of Deep Ultraviolet Emission.

Coherent deep ultraviolet (DUV) light sources are crucial for various applications such as nanolithography, biomedical imaging, and spectroscopy. DUV light sources can be generated by using conventional nonlinear optical crystals (NLOs). However, NLOs are limited by their bulky size, inadequate transparency at the DUV regime, and stringent phase-matching requirements for harmonic generation. Recently, dielectric metasurfaces support high Q-factor resonances and offer a promising approach for efficient harmonic generation at short wavelengths. In this study, we demonstrated a crystalline silicon (c-Si) metasurface simultaneously exciting modal phase-matched bound states in the continuum (BIC) resonance at the fundamental wavelength of 840 nm with a higher degree of freedom for precise control of the BIC resonance and a plasmonic resonance at the wavelength of 280 nm in the DUV to enhance third harmonic generation (THG). We experimentally achieved a Q-factor of ∼180 owing to the relatively large refractive index of the c-Si and the geometric symmetry breaking of the structure. We realized THG at a wavelength of 280 nm with a power of 14.5 nW by using a peak power density of 15 GW/cm2 excitation. The measured THG power is 14 times higher than the state-of-the-art THG dielectric metasurfaces using the same peak power density in the DUV regime, and the maximum obtained THG power enhancement factor is up to 48. This approach relies on the significant third-order nonlinear susceptibility of c-Si, the interband plasmonic nature of the c-Si in the DUV, and the strong field confinement of BIC resonance to boost overall nonlinear conversion efficiency to 5.2 × 10-6% in the DUV regime. Our work shows the potential of c-Si BIC metasurfaces for developing efficient and ultracompact DUV light sources using high-efficacy nonlinear optical devices.

Tunable Nonlinear Optical Properties Based on Metal–Organic Framework Single Crystals

AbstractSolid‐state hybrid materials with designability in topology and tunable photo‐responsiveness hold great promise for multitudinous applications from optoelectronics to information storage/communication. However, the judicious design and synthesis of metal–organic frameworks (MOFs) with intrinsically custom‐made nonlinear optical (NLO) properties including multiple photon absorption and harmonic generation effects suitable for miniaturized devices remain highly challenging. Herein, the design and synthesis of a novel pillared framework named after Zn‐TCPE‐DPNI MOF coordinated by zinc ions (Zn2+), aggregation induced emission (AIE) featured [1,1′‐biphenyl]‐4‐carboxylic acid (H4TCPE), and N,N′‐di(4‐pyridyl)‐1,4,5,8‐naphthalenetetracarboxydiimide (DPNI) are reported. The highly ordered Zn‐TCPE‐DPNI MOF single crystal exhibits tunable NLO responses by switching incident excitation wavelengths of a femtosecond laser from 900 to 1500 nm. The noticeable transformation from two‐ or three‐photon excited photoluminescence (2PL or 3PL) to the concurrent occurrence of 3PL and third harmonic generation (THG), and eventually to the mere emergence of THG with a high effective susceptibility χ(3) (3ω) of 2.9 × 10−12 esu is observed. This study paves a novel avenue for the design and synthesis of photoluminescent MOF crystals with tunable NLO responses toward the fabrication of multifunctional NLO devices targeted for optoelectronics and information communication.

Resonant third-harmonic generation driven by out-of-equilibrium electron dynamics in sodium-based near-zero index thin films

Abstract We investigate resonant third-harmonic generation in near-zero index thin films driven out-of-equilibrium by intense optical excitation. Adopting the Landau weak coupling formalism to incorporate electron–electron and electron–phonon scattering processes, we derive a novel set of hydrodynamic equations accounting for collision-driven nonlinear dynamics in sodium. By perturbatively solving hydrodynamic equations, we model third-harmonic generation by a thin sodium film, finding that such a nonlinear process is resonant at the near-zero index resonance of the third-harmonic signal. Thanks to the reduced absorption of sodium, we observe that third-harmonic resonance can be tuned by the impinging pump radiation angle, efficiently modulating the third-harmonic generation process. Furthermore, owing to the metallic sodium response at the pump optical wavelength, we find that the third-harmonic conversion efficiency is maximised at a peculiar thin film thickness where evanescent back-reflection provides increased field intensity within the thin film. Our results are relevant for the development of future ultraviolet light sources, with potential impact for innovative integrated spectroscopy schemes.

Enhanced terahertz third-harmonic generation based on the graphene-assisted meta-grating structure

The nonlinear response of optical materials provides a valuable approach for optical switching and nonlinear frequency conversion. However, the nonlinear responses of bulk crystals are often very weak, requiring higher pump energy for pumping. In this work, we investigate the significant enhancement of third harmonic generation (THG) at terahertz frequencies using an ultra-thin nonlinear meta-grating metasurface assisted by graphene strips. In this structure, the incident pump light experiences strong confinement and enhancement along the graphene surface caused by the generation of strongly localized surface plasmon resonances. Utilizing the significant third-order nonlinear conductivity of graphene, it becomes possible to achieve high THG conversion efficiency even at low pump intensities. The research results indicate that, at low incident intensity of 10 kW/cm2, the third harmonic wave conversion efficiency can reach approximately 2.8 %. We also thoroughly investigate the impact of meta-grating structural parameters, graphene Fermi level, incident angle, and pump light intensity on THG operation characteristics. Our study findings provide an effective approach for greatly boosting the THG conversion efficiency in the terahertz frequency bands, opening new avenues in the development of novel compact frequency converters and modulators that are emerging in terahertz chip integration and nonlinear devices.

LGYSB:Nd─High-Performance Lasing in the Near-Infrared Region.

Three incongruent melting LawNdxGdyYzSc4-w-x-y-z(BO3)4 (LGYSB:Nd) crystals with different Y concentrations (z = 0.15, 0.05, and 0.025) have been grown by the Czochralski method for the first time. The LGYSB:Nd-type crystals exhibit an acentric structure similar to that of the natural mineral huntite CaMg3(CO3)4, with space group R32. The composition of the LGYSB:Nd_3 (z = 0.025) crystal grown from the starting melt composition La0.628Gd0.547Y0.025Nd0.05Sc2.75(BO3)4 was measured by inductively coupled plasma mass spectrometry method, and it was found to be La0.6794Gd0.4105Y0.0178Nd0.0381Sc2.8542(BO3)4. The transversal spatial distribution of the refractive index in the LGYSB:Nd_3 crystal was investigated. Third-order nonlinear optical susceptibility χ(3) of the LGYSB:Nd_3 crystal was determined from third-harmonic generation experiments with ultrashort (fs) laser pulses. The optical transmission spectrum was measured in the range of 200-2000 nm. The absorption cross-section at 808 nm in σ-polarization was determined to be 1.18 × 10-19 cm2 for the LGYSB:Nd_3 crystal. The 10K absorption spectra revealed that the Nd3+ ions occupy only La3+ cationic sites in the LGYSB host matrix. The emission cross-section at 1064 nm in σ-polarization was determined to be σem(σ) = 1.74 × 10-19 cm2 for the LGYSB:Nd_3 crystal. The fluorescence lifetime was found to be τ = 115 μs for all of the LGYSB:Nd crystals. The LGYSB:Nd_3 laser was operated at an emission wavelength of 1062 nm with very high slope efficiencies of ηsa = 0.74 and ηsa = 0.64 in quasi-cw and cw regimes, respectively.

Third harmonic generation microscopy of magnetic domains in garnet films

Nonlinear optical microscopy is a powerful non-destructive technique that allows to study a wide range of phenomena. Optical third harmonic generation (THG) is mostly known by its applications in investigation of biological structures, while magneto-optical effects in THG are not well recognized. Here we demonstrate high efficiency of the THG probe in studies of magnetic domain structure of epitaxial garnet films. We show that in spite of relatively small values of the magneto-optical effect at the THG wavelength, the THG microscopy may be efficient for the characterization of magnetic surface domains if the THG wavelength falls in the absorption band of a medium. Moreover, the in-depth sensitivity of this probe may be higher as compared to the case of the second harmonic generation microscopy.

Resonantly enhanced second- and third-harmonic generation in dielectric nonlinear metasurfaces

Resonantly enhanced second- and third-harmonic generation in dielectric nonlinear metasurfaces

Strong anisotropic third-harmonic generation in layered violet phosphorus.

We demonstrate that layered violet phosphorus, an emerging 2D semiconductor, undergoes strong anisotropic third-harmonic generation (THG). Polarization dependence of in-plane THG presents a cruciate-flower-shaped curve. Through theoretical modeling of the in-plane THG response, done by considering crystalline symmetry of violet phosphorus, we successfully quantify four non-zero third-order nonlinear optical susceptibility tensor elements. From control experiments, the magnitude of third-order nonlinear optical susceptibility |χ3| is calculated to be about 4.0 × 10-19 m2 V-2, which is comparable to those of conventional 2D layered semiconductors. These results indicate that the layered violet phosphorus can serve as an ideal building block for nonlinear optical applications.

Probing compositional engineering effects on lead-free perovskite-inspired nanocrystal thin films using correlative nonlinear optical microscopy.

We introduce the use of correlative third-harmonic generation and multiphoton-induced luminescence microscopy to investigate the impact of manganese (Mn) doping on bismuth (Bi)-based perovskite-inspired nanocrystal thin films. The technique was found to be extremely sensitive to the microscopic features of the perovskite film and its structural compositions, allowing the unambiguous detection of compositionally different emitters in the perovskite film and manipulation of their nonlinear optical responses. Our work unveils a new way to investigate, manipulate, and exploit perovskite-inspired functional materials for nonlinear optical conversion at the nanoscale.