Large Nonlinear Coefficient Research Articles

Broadband nonlinear Bragg diffraction from self-assembled structures in potassium tantalate niobate crystals

Nonlinear optical process is a key technology to realize optical communication. Potassium tantalate niobate (KTa1−xNbxO3, KTN) crystals with large nonlinear optical coefficients are potential functional materials for realizing χ2 nonlinear optical processes. However, to accurately modulate the nonlinear optical signals of KTN crystals, the relationship between their second harmonic generation (SHG) properties and ferroelectric domain structures needs to be further investigated. Here, we report the special SHG processes generated by self-assembled structures in KTN crystals. Multimode quasi-phase matching and broadband nonlinear Bragg diffraction are achieved with the changing of polarizations and wavelengths of the fundamental wave. The physical processes behind the multi-polarization and multi-wavelength SHG properties of the KTN crystals are revealed. Our results about the multi-polarization and multi-wavelength SHG properties of KTN crystals will provide guidance for the design and realization of multimode nonlinear optical processes.

Polymer functionalized antimony sulfide quantum dots for broadband optical limiting.

The rapid development of zero-dimensional quantum dots-based nanotechnology has motivated the design and synthesis of novel nano-functional materials for optoelectronic and photonic devices in recent years. Antimony sulfide (Sb2S3) quantum dots (SQDs), with an average diameter of 3.22 nm, were prepared via a top-down liquid ultrasonication exfoliation technique. Highly soluble poly(N-vinylcarbazole)-covalently functionalized SQDs (SQDs-PVK) were synthesized in situ by reversible addition fragmentation chain transfer polymerization, and embedded into a non-optically active poly(methylmethacrylate) (PMMA) matrix giving the SQDs-PVK/PMMA film. The annealed SQDs-PVK/PMMA film showed exceptional nonlinear optical performance, with large nonlinear absorption coefficients of 713.71 cm GW-1 at 532 nm and 913.60 cm GW-1 at 1064 nm, and small limiting thresholds of 1.44 J cm-2 at 532 nm and 1.08 J cm-2 at 1064 nm. These advantages make SQDs-PVK one of the promising candidates for a broadband optical limiter in both the near-infrared and visible ranges.

Efficient second-harmonic generation in a lithium niobate metasurface governed by high-Q magnetic toroidal dipole resonances.

Lithium niobate (LN) is an excellent nonlinear optical material due to its large nonlinear coefficient, low loss, and broad optical transparency window. So, it is widely used in the generation of nonlinear harmonics. Magnetic toroidal dipole (MTD) resonance is a special optical resonance mode, which can effectively localize the light field inside the device, thus enhancing the nonlinear effects of the materials. In this work, we numerically study the second-harmonic generation (SHG) effect of the LN metasurface based on the MTD mode with a high quality factor (Q-factor). The designed LN nanorod dimer metasurface supports high Q-factor MTD guided mode resonances (GMRs), which are excited by varying the center spacing of the two nanorods, and the Q-factor can be controlled by the offset distance. The excited MTD can effectively confine the electric field within the device, which enables the LN metasurface SHG conversion efficiency to reach 1.15 × 10-2. In addition, by adjusting the structural parameters, it is possible to effectively modulate the wavelength and conversion efficiency of the SHG. Our results provide a new route for high-quality nonlinear light sources.

Interfacial Synthesis of Two‐Dimensional Porphyrin Polymer Films with Large Optical Nonlinearity

Two‐dimensional polymers (2DPs) and their layer‐stacked 2D covalent organic frameworks have recently emerged as nonlinear optical (NLO) materials for potential applications in optics. However, the chemistry for designing third‐order NLO 2DP films with large nonlinear absorption coefficient (β) has remained a mystery. Herein, three highly crystalline porphyrin‐integrated 2D polyimines (named as 2DPI‐Zn‐Azo, 2DPI‐2H‐Azo, and 2DPI‐Zn), which are homogeneous films showing large lateral areas over cm2, uniform transparency, and thickness of tens of nanometers are reported. Particularly, the 2DPI‐Zn‐Azo film comprising zinc porphyrin and –NN– displays a large saturable absorption under 532 nm and the highest β (−1.88 × 105 cm GW−1) among the three 2D polyimines, that is also 2–5 orders of magnitude higher than the state‐of‐art performance of photoactive small molecules, porphyrin‐integrated 2DPs, and inorganic 2D materials. Control experiments in combination with theoretical calculation discover that the embedding of metal centers and –NN– results in highly delocalized π‐electrons and narrow bandgap in 2DPI‐Zn‐Azo, which enables fast transfer of the photogenerated electrons after the light‐excited charge separation, thus boosting the NLO performance. This work opens up a new path for the construction of highly efficient third‐order NLO film materials, and pushes the development of 2DPs for optics and optoelectronics.

Phase-matched five-wave mixing in zinc oxide microwire

Abstract High-order wave mixing in solid-state platforms gather increasing importance due to the development of advanced lasers and integrated photonic circuit for both classical and quantum information. However, the high-order wave mixing is generally inefficient in solids under weak pump. Here, we observed the presence of phase matching of five-wave mixing (5WM) propagating in a zinc oxide (ZnO) microwire. The 5WM signal is enhanced by 2–3 orders of magnitude under the phase matching conditions, reaching an absolute conversion efficiency of 1.7 × 10−13 when the peak pumping power density is about 106 W/cm2. The propagation of multiple nonlinear signals, including sum frequency generation, third harmonic generation, four-wave mixing etc., benefited from both the large nonlinear coefficients and the wide transparent window of ZnO, implies the possibility of developing cascaded nonlinear process under higher pumping. This study enriches the ZnO platform for integrated nonlinear nanophotonics.

High second-order nonlinearity in single-domain tetragonal PMN-PT single crystal

Recently, Pb(Mg1/3Nb2/3)O3-xPbTiO3 (PMN-xPT) single crystals present tremendous potential in optical applications such as Q-switches and invisible robotic devices because they possess high electro-optic properties and perfect transparency simultaneously. However, due to the difficulties in testing and sample preparation, the nonlinear optical properties of PMN-PT single crystals have not been reported yet, which poses a bottleneck for exploring its nonlinear application. In this work, a large second-order nonlinear coefficient (d31 ∼ 77.9 pm V−1) of single domain PMN-0.39PT single crystal has been revealed, which is times times higher than the maximum nonlinear coefficient of commercial LiNbO3 single crystal (d33 = 25.4 pm V−1). The complete set of nonlinear coefficients of the sample has been determined by second harmonic generation microscopy. This work presents the promising nonlinear optical property in PMN-PT single crystals and opens a door for designing high-performance nonlinear optical devices.

Strong nonlinear optical limiting of resin composed by carbon nanotubes

The development of solid-state nonlinear optical limiting (NOL) materials is crucial for advancing the practicality in the field of optical limiting. In this paper, we innovatively prepare a new solid NOL material which is spiral carbon nanotubes doped epoxy resin (SCNTs-doped ER, SER) with a simple physical mixing method, and achieve an excellent nonlinear optical limiting performance. We experimentally measured optical limiting of SER with different SCNTs concentrations (0.14, 0.28, and 0.43 mg/mL) and obtained the nonlinear absorption coefficient, nonlinear refractive index, and third-order nonlinear susceptibility at the wavelength 1064 nm. Z-scan experiment results show that the SER exhibits a large nonlinear absorption coefficient (5.07 ± 0.38) × 10−9 m/W. We also measure the transmittance of the SER to evaluate its nonlinear optical limiting performance. For the SER with 0.43 mg/mL concentration, the linear transmittance and minimum transmittance with NOL effects at 1064 nm are 54.8% and 26.2%, respectively. In addition, the SER also has prominent features such as a high damage threshold and easy fabrication, indicating that the SER is a promising solid material for nonlinear optical limiting.

Third-order nonlinear optics and optical limiting of phenanthrenone derivatives

Organic nonlinear optical materials have attracted much attention due to their large nonlinear optical coefficients and ultrafast response speeds, as well as their potential applications in optical limiting (OL). Among them, nonlinear optical materials with phenanthrenone as the backbone are consistently understudied. We have successfully realized the transformation of organic small molecules in the nonlinear optical direction by replacing the carbonyl group on the structure of phenanthrenone with a malononitrile group. The nonlinear optical properties of CN-2 were investigated under different excitation conditions at 532 nm and the kinetic process of nonlinear optics was analyzed by transient absorption spectroscopy. In addition, we also investigated the OL properties of CN-2, and the OL experiments showed that CN-2 with a lower OL threshold has superior OL properties than C60.

Porous nano-grained cuprous selenide (Cu2Se) for mid-infrared photonics

Recently, mid-infrared photonics has attracted tremendous attention for various applications. To address the dilemma of the limited variety of materials for mid-infrared photonics, the mid-infrared optical modulation characteristics of the porous nano-grained cuprous selenide (Cu2Se) were investigated for the first time. The large effective nonlinear absorption coefficient, large modulation depth, and low saturation absorption intensity at 2.3 μm indicate that the porous nano-grained Cu2Se were promising saturable absorbers for the generation of Q-switched pulsed laser in the mid-infrared regime. As an application, the Tm:GdVO4 passively Q-switched laser operating on the 3H4 → 3H5 Tm3+ transition was achieved for the first time by using the prepared porous nano-grained Cu2Se as the saturable absorber. The minimum pulse duration and the maximum repetition rate of the stable Q-switched pulse train were 440 ns and 76.9 kHz, respectively. Our results demonstrated that the porous nano-grained Cu2Se was a promising candidate for the mid-infrared photonic applications.

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.

Improving fourth harmonic generation performance by elevating the operation temperature of ADP crystal.

In current inertial confinement fusion (ICF) facilities, potassium dihydrogen phosphate (KH2PO4, KDP) type crystals are the only nonlinear optical (NLO) materials that can satisfy the aperture requirement of the ICF laser driver. Ammonium dihydrogen phosphate (NH4H2PO4, ADP) crystal is a typical isomer of KDP crystal, with a large nonlinear optical coefficient, high ultraviolet transmittance, and large growth sizes, which is an important deep ultraviolet (UV) NLO material. In this paper, we investigated the effect of ADP temperature on its fourth-harmonic-generation (FHG) performance. When the temperature of the ADP crystal was elevated to 48.9 °C, the 90° phase-matched FHG of the 1064 nm laser was realized. Compared with the 79° phase-matched FHG at room temperature (23.0 °C), the output energy at 266 nm, conversion efficiency, angular acceptance, and laser-induced damage threshold (LIDT) increased 113%, 71%, 623%, 19.6%, respectively. It shows that elevating ADP temperature is an efficient method to improve its deep UV frequency conversion properties, which may also be available to other NLO crystals. This discovery provides a very valuable technology for the future development of UV, deep UV lasers in ICF facilities.

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.

Significantly improved giant dielectric properties and enhanced nonlinear coefficient of Ni2+ doped CaCu3Ti4O12/CaTiO3 composites

CaCu3-xNixTi4O12/CaTiO3 ceramic composites were fabricated using initial Ca2Cu2-xNixTi4O12 compositions (x = 0, 0.05, 0.10, and 0.20) to improve the dielectric properties (DPs) of the CaCu3Ti4O12 ceramics. CaCu3Ti4O12 and CaTiO3 phases were confirmed. Microstructural analysis and Rietveld refinement showed that the Ni2+ dopant might substitute the Cu2+ sites of the CaCu3Ti4O12 structure. The average grain sizes of CaCu3Ti4O12 (4.1–5.6 μm) and CaTiO3 (1.2–1.4 μm) changed slightly with the Ni2+ doping concentration. The best DPs were obtained for the CaCu3-xNixTi4O12/CaTiO3 with x = 0.2. The loss tangent was significantly reduced by an order of magnitude compared to that of the undoped composite, from tanδ∼0.161 to ∼0.016 at 1 kHz, while the dielectric permittivity slightly decreased from ε′∼5.7 × 103 to ∼4.0 × 103. Furthermore, the temperature dependence of ε′ could be improved by doping with Ni2+. The improved DPs were caused by the enhanced electrical responses of the internal interfaces, which resulted in enhanced non–Ohmic properties. The largest nonlinear coefficient (α∼7.6) was obtained for the CaCu3-xNixTi4O12/CaTiO3 with x = 0.05. Impedance spectroscopy showed that the CaCu3-xNixTi4O12/CaTiO3 composites consisted of semiconducting and insulating components. The DPs of CaCu3-xNixTi4O12/CaTiO3 were explained based on the space−charge polarization at the active−interfaces.

Enhancement of second-order optical nonlinearities and nanoscale periodic domain patterning in ferroelectric boron-substituted aluminum nitride thin films

The discovery and development of CMOS-compatible, nonlinear optical materials is essential to produce integrated photonic devices with advanced functionalities. AlN is a strong candidate for on-chip device demonstration due to its intrinsic second-order optical nonlinearities, large bandgap, and well-established fabrication techniques. However, AlN is not easily phase matched for the largest coefficient d33; the coefficients that could potentially be dispersion phase-matched, d31 and d15, have weak nonlinearities. This work investigates ferroelectric Al1-xBxN (x = 0 to 0.11) for viability as a large bandgap nonlinear optical material with unique suitability towards ultraviolet light generation using second harmonic generation. The linear and nonlinear optical properties are characterized accounting for material anisotropy. With increasing B concentration, a large enhancement from near negligible values to d31 = 0.9 ± 0.1 pm/V and d15= 1.2 ± 0.1 pm/V is observed. This compares favorably to other large bandgap materials like β-Ba(BO2)2, where the largest nonlinear coefficient is d22 ∼ 2.3 pm/V at 800 nm. This is accompanied by a change in the bandgap from 6.1 eV to 5.8 eV as B substitution goes from 0 to 11%. A periodically poled, quasi-phase-matched ferroelectric domain pattern with 400 nm domain size and a wall roughness of <16 nm is demonstrated.

Nonlinear optical properties of PVD-grown Cr2Te3 film and its nonlinear switching application

Recently, two-dimensional (2D) nanomaterials have been investigated extensively in the field of nonlinear photonics. Cr2Te3, which is one of the 2D transition metal chalcogenides, has garnered attention in the field of spintronics and optoelectronics because of its fascinating magnetic and optical properties. Despite its potential in optoelectronics, Cr2Te3 has rarely been studied in the field of nonlinear photonics. This study investigates the nonlinear optical responses of nanoscale-layered Cr2Te3 films grown by physical vapor deposition at telecommunication wavelengths. A large nonlinear absorption coefficient of –(1.43 ± 0.06) × 105 cm/GW and a nonlinear refractive index of –1.22 ± 0.04 cm2/GW at 1560 nm obtained through Z-scan measurements indicate that the Cr2Te3 film shows saturable absorption and self-defocusing properties at telecommunication wavelengths. Density functional theory calculation show that Cr2Te3 is suitable for broadband optical device. The potential of the nanoscale-layered Cr2Te3 film as a base medium for a nonlinear optical switch was evaluated by fabricating a saturable absorption mirror (SAM). Stable Q-switched pulses with a maximum repetition rate of 33.35 kHz and minimum temporal width of 2.62 μs were readily achieved from a fiber laser cavity incorporating the SAM.

Highly sensitive biosensor based on a microstructured photonic crystal fibre for alcohol sensing

A microstructure alcohol biosensor has been proposed to operate in the wavelength range of 0.8 to 2.0 µm for the sensing of propanol, butanol, and pentanol, unveiling impressive results of relative sensitivity and confinement loss. The results are achieved by implementing closely arranged cladding air holes of 3 rings with a single elliptical core hole for analyte infiltration. Performance evaluation of the sensor was conducted using COMSOL Multiphysics software and yields relative sensitivity of 96.75%, 89.60%, and 82.02% for propanol, butanol, and pentanol, respectively, and confinement losses of 5.49 × 10−12 dB/m for propanol, 1.98 × 10−12 dB/m for butanol, and 9.36 × 10−13 dB/m for pentanol. Other optical parameters have also been analysed that recorded effective refractive index, high power fraction, low birefringence, small effective area, and large nonlinear coefficients. The proposed biosensor is eligible for practical application in alcohol sensing with these results. Moreover, this proposed biosensor is suitable as a supercontinuum source in optical communication systems because of the high nonlinear coefficients.

Tunable phase-mismatched mid-infrared difference-frequency generation between 6 and 17 µm in CdTe.

In parametric conversion, phase-matching techniques such as birefringence and quasi phase-matching (PM) with the designed crystal angle or periodically poled polarities are employed to fulfill the requirement of momentum conservation. However, directly using phase-mismatched interactions in nonlinear media with large quadratic nonlinear coefficient remains unheeded. Here, for the first time to the best of our knowledge, we study the phase-mismatched difference-frequency generation (DFG) in an isotropic cadmium telluride (CdTe) crystal, with the comparison of other DFG processes based on birefringence-PM, quasi-PM, and random-quasi-PM. Long-wavelength mid-infrared (LWMIR) phase-mismatched DFG with an ultra-broadband spectral tuning range of 6-17 µm based on CdTe is demonstrated. Thanks to the giant quadratic nonlinear coefficient (∼109 pm/V) and good figure of merit in the parametric process, the output power up to 100 µW is obtained, which is comparable to or even better than the DFG output from a polycrystalline ZnSe with the same thickness facilitated by random-quasi-PM. A proof-of-concept demonstration in gas sensing of CH4 and SF6 is conducted based on the phase-mismatched DFG as a typical application. Our results demonstrate the feasibility of phase-mismatched parametric conversion in producing useful LWMIR power and ultra-broadband tunability in a simple and convenient way without the necessity of controlling the polarization, phase-matching angle, or pole periods, which could find applications in the fields of spectroscopy and metrology.

Wafer-scale heterogeneous integration of thin film lithium niobate on silicon-nitride photonic integrated circuits with low loss bonding interfaces.

Silicon nitride (Si3N4) is a versatile waveguide material platform for CMOS foundry-based photonic integrated circuits (PICs) with low loss and high-power handling. The range of applications enabled by this platform is significantly expanded with the addition of a material with large electro-optic and nonlinear coefficients such as lithium niobate. This work examines the heterogeneous integration of thin-film lithium-niobate (TFLN) on silicon-nitride PICs. Bonding approaches are evaluated based on the interface used (SiO2, Al2O3 and direct) to form hybrid waveguide structures. We demonstrate low losses in chip-scale bonded ring resonators of 0.4 dB/cm (intrinsic Q = 8.19 × 105). In addition, we are able to scale the process to demonstrate bonding of full 100-mm TFLN wafers to 200-mm Si3N4 PIC wafers with high layer transfer yield. This will enable future integration with foundry processing and process design kits (PDKs) for applications such as integrated microwave photonics and quantum photonics.

Modular Design of a Polymer-Bilayer-Based Mechanically Compliant Worm-Like Robot.

Soft earthworm-like robots that exhibit mechanical compliance can, in principle, navigate through uneven terrains and constricted spaces that are inaccessible to traditional legged and wheeled robots. However, unlike the biological originals thatthey mimic, most of the worm-like robots reported to date contain rigid components that limit their compliance, such as electromotors or pressure-driven actuation systems. Here, a mechanically compliant worm-like robot with a fully modular body that is based on soft polymers is reported. The robot is composed of strategically assembled, electrothermally activated polymer bilayer actuators, which are based on a semicrystalline polyurethane with an exceptionally large nonlinear thermal expansion coefficient. The segments are designed on the basis of a modified Timoshenko model, and finite element analysis simulation is used to describe their performance. Upon electrical activation of the segments with basic waveform patterns, the robot can move through repeatable peristaltic locomotion on exceptionally slippery or sticky surfaces and it can be oriented in any direction. The soft body enables the robot to wriggle through openings and tunnels that are much smaller than its cross-section.

Universality in nonlinear passage through the miscible-immiscible phase transition in two component Bose-Einstein condensates

In this study, we investigate the formation of domain defects and the universal critical real-time dynamics in a two-component Bose-Einstein condensate with nonlinear quenching across the miscible-immiscible phase transition. By analyzing the Bogoliubov excitations, we obtain the power-law relations among the defect density, the phase transition delay and the quench time near the phase transition. Moreover, by simulating the real-time dynamics across the miscible-immiscible phase transition, we clearly show the formation of domain defects and the delay of the phase transition. Furthermore, we find that the domain defects are suppressed by large nonlinear coefficients and long quench times. To accurately characterize the domain defects, we quantify the defect excitations using the correlation length and the domain number. In addition, by combining the power-law relations between the phase transition delay and the quench time, we extract the critical exponents for different nonlinear coefficients. Our study not only confirms that the critical exponents do not sensitively depend on the nonlinear quenches but also provides a dynamic path toward the suppression of nonadiabatic excitation.