Phase-matching Wavelength Research Articles

K0.9Rb2.1B8PO16: Design and Synthesis of a Deep-Ultraviolet Nonlinear Optical Crystal with Balanced Performance Derived from π-Conjugated and Non-π-Conjugated Groups.

A new deep-ultraviolet (DUV) nonlinear optical (NLO) material K0.9Rb2.1B8PO16 (KRBPO) has been designed and synthesized by adjusting the B/P molar ratio to 8:1. The KRBPO crystals were synthesized by a flux method and crystallized in noncentrosymmetric (NCS) and polar space group Cc. This compound exhibits a double-layer structure in which the A layer is composed of [B2O5] and [BO4] units and the B layer is formed by interconnected [B3O7] and [BO3] groups, and the two layers are connected by [PO4] tetrahedron. The theoretical calculations and experiments show that the synergistic interaction of π-conjugated and non-π-conjugated units leads to relatively well-balanced NLO properties of the title compound, including moderated SHG (0.7 × KDP), short UV cutoff edge (λcutoff < 190 nm), and a large band gap of 6.16 eV. Specifically, the coplanar arrangement of B-O groups in double-layer makes the KRBPO display a large birefringence (0.075@532 nm) and enables the shortest phase-matched wavelength to reach an important laser output wavelength of 266 nm.

Concurrent phase-matchings for multi-wavelength conversion in coupled dual waveguides

Thin film lithium niobate, as a highly promising integrated photonics platform, has emerged as an ideal material platform for wavelength conversion owing to its exceptional second-order nonlinear characteristics. Here, we present the first demonstration of concurrent phase-matchings for multi-wavelength conversion in coupled thin film lithium niobate waveguides without poling technique. In the coupled dual waveguide system, employing modal phase-matching, we validate three effective phase-matching conditions for second harmonic generation, arising from additional momentum compensation due to the coupling of waveguides. Simultaneously, we confirm that phase-matching wavelengths can be tuned by adjusting the gap between waveguides. The concurrent phase-matchings in coupled dual waveguide systems can be readily extended to other nonlinear optical processes, such as difference frequency generation and spontaneous parametric down conversion. Our work contributes to advancing the exploration of efficient on-chip nonlinear optical processes within the realms of nanophotonics and quantum optics.

Generation of multiple user-defined dispersive waves in a silicon nitride waveguide

The quest for a wide and bright supercontinuum source has received significant attention, addressing pivotal challenges in ultra-fast spectroscopy, imaging, and frequency metrology. Among the diverse optical nonlinear mechanisms steering supercontinuum generation, dispersive waves emerge as crucial contributors, providing heightened spectral intensity, wavelength tunability, and superior temporal coherence. Nevertheless, their generation is tightly bound by waveguide geometry, limiting both their numbers and the wavelengths at which they manifest. In this paper, we demonstrate the controlled generation of multiple dispersive waves in fundamental optical transverse mode by leveraging quasi phase-matching in an integrated silicon nitride (Si3N4) waveguide. This approach involves modulating the group velocity dispersion through varying the width of the Si3N4 waveguide crossing anomalous and normal dispersion, which facilitates the creation of diverse dispersive waves in fundamental transverse electromagnetic (TE) polarization at multiple phase-matched wavelengths. A wide nonlinear optical spectral broadening surpassing conventional approaches is achieved with good temporal and spatial coherence. Remarkably, the generation of the multiple dispersive waves and the supercontinuum is achieved by a 190-fs pulse duration pump with peak power as low as 110 W (24 pJ). This work offers flexibility to manipulate dispersive waves in an integrated platform beyond current dispersion engineering. It represents a significant step forward in developing an integrated broadband source with a user-defined spectral shape, accomplished with minimal pump power requirements.

Phase-matched third-harmonic generation in silicon nitride waveguides.

Third-harmonic generation (THG) in silicon nitride waveguides is an ideal source of coherent visible light, suited for ultrafast pulse characterization, telecom signal monitoring and self-referenced comb generation due to its relatively large nonlinear susceptibility and CMOS compatibility. We demonstrate third-harmonic generation in silicon nitride waveguides where a fundamental transverse mode at 1,596 nm is phase-matched to a TM02 mode at 532 nm, confirmed by the far-field image. We experimentally measure the waveguide width-dependent phase-matched wavelength with a peak-power-normalized conversion efficiency of 5.78 × 10-7 %/W2 over a 660-μm-long interaction length.

Asymmetric dual-core liquid crystal channel-based tunable mode converter

In this work, a higher order-to-fundamental mode converter is reported and analyzed based on an asymmetric dual channel waveguide (ADC-WG) on silicon. In the reported structure, one of the two waveguides is infiltrated with nematic liquid crystal (NLC) material to add temperature tunability while the other one is a solid BK7 waveguide. The modal characteristics are obtained using the full vectorial finite difference method (FVFDM). In addition, the structural parameters and optical characteristics of the employed materials are investigated to achieve good wavelength selectivity with a short device length (LD). Thus, a compact mode converter that can work at different wavelengths including the telecommunication wavelength i.e., 1.55 μm with LD ~ 482.31 μm and a low crosstalk of − 19.86 dB is presented. To prove the thermal tunability of the suggested mode converter, its operation is tested through a temperature range between 20 and 35 °C and the results show that the mode conversion process is achieved at each temperature with different phase matching wavelengths (λPMW) but with quite similar coupling length (LC). The proposed device can therefore be effectively utilized in integrated photonic circuits.

Highly sensitive plasmonic-grating PCF biosensor for cancer cell detection

Highly sensitive biosensor based on D-shaped photonic crystal fiber (PCF) with plasmonic grating is introduced and analyzed. The suggested structure is tested using four different grating structures (rectangular, triangular, circular, or elliptical) on the polished surface of the D-shaped PCF. The sensing operation depends on surface plasmon resonance mechanism where the analyte refractive index (RI) is utilized to control the coupling between the core mode and surface plasmon mode via phase matching phenomenon. Rhodium is employed as a plasmonic material to induce the SPMs. The resonance (i.e., phase matching) wavelength is a function of the analyte RI. The geometrical parameters of the proposed structure are optimized using full vectorial finite element method to enhance the sensor sensitivity. The proposed biosensor can be utilized in the detection of different cancerous Basel, Breast and Cervical cells. The performance of the reported biosensor is investigated in terms of sensitivity, linear response, and fabrication tolerance. The reported biosensor has high sensitivities of 19,750 nm/RIU, 20,428 nm/RIU and 20,041 nm/RIU for the detection of Basel, Breast and Cervical cancer cells, respectively. The presented biosensor is a good candidate for biological sample detection and organic chemical sensing.

Li3Na7B4P6O26: a new ultraviolet transparent congruently melting non-linear optical crystal.

The exploration of nonlinear optical crystals with ultraviolet (UV) transparent ranges and easy-to-grow large-size crystals is one of the current research interests. Herein, by combining borate and phosphate groups, a novel congruently melting alkali-mixed metal borophosphate, Li3Na7B4P6O26 (LNBPO) with UV transparency was successfully designed and synthesized using a high-temperature flux method. LNBPO crystallizes in the non-centrosymmetric (NCS) and polar orthorhombic space group Pca21 (no. 29), showcasing interesting (B2P3O13)∞ chains along the c axis. Notably, LNBPO has a moderate second harmonic generation (SHG) response (∼0.38 × KDP) and displays a wide transmission ranging from 0.22 to 3.68 μm, as measured by a [001]-oriented crystal wafer. Furthermore, a high-quality single crystal of LNBPO with sizes up to 14 × 14 × 12 mm3 was grown using the top-seeded solution growth method. The refractive indices of LNBPO were determined by applying the minimum deviation angle method. These results show that LNBPO possesses a phase-matching wavelength as short as 483 nm, indicating its potential as a new UV NLO crystal.

Mg(C3 O4 H2 )(H2 O)2 : A New Ultraviolet Nonlinear Optical Material Derived from KBe2 BO3 F2 with High Performance and Excellent Water-Resistance.

Acquiring high-performance ultraviolet (UV) nonlinear optical (NLO) materials that simultaneously exhibit a strong second harmonic generation (SHG) coefficients, as short as possible SHG phase-matching (PM) wavelength and non-hygroscopic properties has consistently posed a significant challenge. Herein, through multicomponent modification of KBe2 BO3 F2 (KBBF), an excellent UV NLO crystal, Mg(C3 O4 H2 )(H2 O)2 , was successfully synthesized in malonic system. This material possesses a unique 2D NLO-favorable electroneutral [Mg(C3 O4 H2 )3 (H2 O)2 ]∞ layer, resulting in the rare coexistence of a strong SHG response of 3×KDP (@1064 nm) and short PM wavelength of 200 nm. More importantly, it exhibits exceptional water resistance, which is rare among ionic organic NLO crystals. Theoretical calculations revealed that its excellent water-resistant may be originated from its small available cavity volumes, which is similar to the famous LiB3 O5 (LBO). Therefore, excellent NLO properties and stability against air and moisture indicate it should be a promising UV NLO crystal.

KHg4Ga3S9: A Hg-Based Sulfide with Nonlinear-Optical Activity in the A-MII-MIII-Q (A = Alkali Metal; MII = d10 Metal; MIII = Ga, In; Q = S, Se) System.

The search for new high-performance infrared (IR) nonlinear-optical (NLO) materials is a hot topic in the fields of laser chemistry and inorganic solid-state chemistry. Here, a new Hg-based sulfide KHg4Ga3S9 in the family of A-MII-MIII-Q (A = alkali metal; MII = d10 metal; MIII = Ga, In; Q = S, Se) was synthesized. It crystallizes in the orthogonal system of the C2221 structure, which is rare for IR NLO chalcogenides. Its anionic framework {[Hg4Ga3S9]-}∞ is constructed by two types of interconnected helical chains, viz., the inner layer ({[Hg6Ga2S29/3]4/3-}∞) and the outer layer ({[Hg2Ga4S25/3]2/3-}∞). It exhibits a moderate NLO response and a high laser-induced damage threshold. Theoretical calculations indicate that the HgS4 unit accounts for its much larger NLO response compared to RbCd4Ga3S9. The influence of alkali metals and d10 metals on the initial phase-matching wavelength is also discussed. This work provides inspiration for improving the properties of NLO materials' properties.

Target-Driven Design of Deep-UV Nonlinear Optical Materials via Interpretable Machine Learning.

The development of a data-driven science paradigm is greatly revolutionizing the process of materials discovery. Particularly, exploring novel nonlinear optical (NLO) materials with the birefringent phase-matching ability to deep-ultraviolet (UV) region is of vital significance for the field of laser technologies. Herein, a target-driven materials design framework combining high-throughput calculations (HTC), crystal structure prediction, and interpretable machine learning (ML) is proposed to accelerate the discovery of deep-UV NLO materials. Using a dataset generated from HTC, an ML regression model for predicting birefringence is developed for the first time, which exhibits a possibility of achieving fast and accurate prediction. Essentially, crystal structures are adopted as the only known input of this model to establish a close structure-property relationship mapping birefringence. Utilizing the ML-predicted birefringence which can affect the shortest phase-matching wavelength, a full list of potential chemical compositions based on an efficient screening strategy is identified. Further, eight structures with good stability are discovered to show potential applications in the deep-UV region, owing to their promising NLO-related properties. This study provides a new insight into the discovery of NLO materials and this design framework can identify desired materials with high performances in the broad chemical space at a low computational cost.

Zn2BS3Br: An Infrared Nonlinear Optical Material with Significant Dual-Property Enhancements Designed through a Template Grafting Strategy

Developing high-performance infrared nonlinear optical (IR-NLO) materials with high second-harmonic generation (SHG) coefficients (dij) and wide band gaps (Eg) has been a serious challenge owing to the intrinsic negative correlativity between the two key properties. Herein, taking π-delocalized BS3 as core functional motifs (FMs), a template grafting strategy that facilitates dual-property enhancement is proposed and novel thioborates of Zn2BS3Br with target IR-NLO performances are predicted by the first-principles evolutionary algorithm. They not only possess wide band gaps of 3.63–4.05 eV, increasing by 1.0 eV over the benchmark AgGaS2 (AGS, 2.62 eV); moreover, benefiting from the parallel alignments of FMs, five phases exhibit high SHG effects (dij > 1.0 × AGS), particularly I (2.0 × AGS & 3.68 eV) and II (2.2 × AGS & 3.77 eV), in which significant enhancements in dij and Eg can be achieved concurrently, surpassing almost all of the accessible IR-NLO materials. Remarkably, the sufficiently wide band gaps and large birefringence of I and II lead to very short phase-matching wavelengths (λPM = 443.9/370.1 nm), enabling them a dual-waveband application potential, which is rarely found in IR-NLO chalcogenides. In addition, the isomorphic selenides show record high SHG coefficients of 3.8 × AGS in the wide-band-gap range of Eg > 3.0 eV. Therefore, the Zn2BS3Br-family crystals would be promising IR-NLO materials. Profound mechanism explorations conclusively demonstrate the effectiveness of our design strategy.

Highly efficient, modal phase-matched second harmonic generation in a double-layered thin film lithium niobate waveguide.

In this contribution, we numerically investigate second harmonic generation in double-layered lithium niobate on the insulator platform by means of the modal phase matching. The modal dispersion of the ridge waveguides at the C waveband of optical fiber communication is calculated numerically and analyzed. Modal phase matching can be achieved by changing the geometric dimensions of the ridge waveguide. The phase-matching wavelength and conversion efficiencies versus the geometric dimensions in the modal phase-matching process are investigated. We also analyze the thermal-tuning ability of the present modal phase matching scheme. Our results show that highly efficient second harmonic generation can be realized by the modal phase matching in the double-layered thin film lithium niobate ridge waveguide.

Coaxial dual-core dispersion compensation photonic crystal fiber with wavelength-tunable ultrahigh negative dispersion

A coaxial dual-core wavelength-tunable dispersion compensation photonic crystal fiber (WT-DC-PCF) is designed in this paper. The tunable range of 1512–1587 nm with an ultrahigh negative dispersion of − 27315.76 p s / ( n m ⋅ k m ) at 1550 nm has been obtained simultaneously by filling the temperature-sensitive material into the air holes of the WT-DC-PCF. The full width at half-maximum is up to 12.4 nm, and a low confinement loss is always maintained. In addition, the phase-matching wavelength is basically linear with the temperature, which can be accurately adjusted to 1550 nm. Therefore, the proposed WT-DC-PCF is able to be used in achieving complete dispersion compensation in communication systems.

CaBO2F: A novel deep-UV structural template with high nonlinear optical performance induced by electron delocalization

Nonlinear optical (NLO) materials with deep-ultraviolet (deep-UV) phase-matching capability are of current interest owing to their applications in photoelectric technology. The anionic framework, including the microscopic unit, arrangement, and connection mode, is vital to optimizing the contradictory NLO performances. Herein, the polarizability characteristics of low-dimensional anionic frameworks were investigated. Results revealed that the oriented electron delocalization in a specific direction enhances the polarization and optimizes the NLO performance. A new borate fluoride system, namely CaBO2F, was designed via top-down structural prediction methods. In this system, CaBO2F-I, II, and III with low energy have one-dimensional (BO2)∞ anionic frameworks. The first-principles calculations show that CaBO2F-I, II, and III have wide deep-UV band gaps, suitable birefringence (0.076–0.108@1064 nm), and large second harmonic generation coefficients (2.1–2.7 × KH2PO4 (KDP)). Particularly, CaBO2F-I has a short phase-matching wavelength of 195 nm (Heyd-Scuseria-Ernzerhof (HSE06)), which is the first alkaline earth borate fluoride template with one-dimensional (BO2)∞ that reaches deep-UV phase-matching capability. This result offers a new guideline for exploring novel NLO materials.

Design of novel deep-UV nonlinear optical materials with one-dimensional functional module [BO2]∞ chain and fluorine-driven short phase-matching

Design of deep-ultraviolet (deep-UV) nonlinear optical (NLO) materials is urgently needed owing to the lack of high-performance crystals to meet the contradictory criteria of deep-UV transparency, strong NLO response and moderate birefringence to reach deep-UV phase-matching. In this work, a “highly-polymerized units optimizing electron delocalization” strategy was proposed to explore novel types of deep-UV NLO anionic functional module and design new materials. Two novel NLO systems with new NLO anionic functional module-one dimensional [BO2]∞ chains were successfully designed. In total, four LiBO2 (I-IV) and five Li2BO2F (I–V) structures with good thermodynamically and dynamically stable/metastable were obtained by using evolutionary algorithm crystal structure prediction techniques. All these structures contain the [BO2]∞ infinite chains and have deep-UV transparency (< 177.3 nm). LiBO2 (II, IV) and Li2BO2F (I, IV-V) exhibit large NLO response (2.0–2.3 × KH2PO4) and large birefringence (0.093–0.146 @1064 nm). Remarkably, Li2BO2F–I possesses an extremely short phase-matching wavelength about 159 nm, which is beneficial from the introduction of fluorine to maintain the superior functional module [BO2]∞ and optimize the optical properties. The results indicate that [BO2]∞ can be as a new deep-UV NLO functional module, this work provides an insight into the design of new deep-UV compound with outstanding NLO performances.

(NH4)3B11PO19F3: a deep-UV nonlinear optical crystal with unique [B5PO10F]∞ layers.

Deep-ultraviolet (DUV) nonlinear optical (NLO) crystals that can extend the output range of coherent light below 200 nm are pivotal materials for solid-state lasers. To date, KBe2BO3F2 (KBBF) is the only usable crystal that can generate DUV coherent light by direct second harmonic generation (SHG), but the layered growth habit and toxic ingredients limit its application. Herein, we report a new fluoroborophosphate, (NH4)3B11PO19F3 (ABPF), containing four different functional units: [BO3], [BO4], [BO3F] and [PO4]. ABPF exhibits a KBBF-like structure while eliminating the limitations of KBBF crystal. The unique [B5PO10F]∞ layers enhance ABPF’s performance; for example, it has a large SHG response (1.2 × KDP) and a sufficient birefringence (0.088 at 1064 nm) that enables the shortest phase-matching wavelength to reach the DUV region. Meanwhile, the introduction of strong B-O-P covalent bonds decreases the layered growth habit. These findings will enrich the structural chemistry of fluoroborophosphate and contribute to the discovery of more excellent DUV NLO crystals.

Cryogenic electro-optic modulation in titanium in-diffused lithium niobate waveguides

Lithium niobate is a promising platform for integrated quantum optics. In this platform, we aim to efficiently manipulate and detect quantum states by combining superconducting single photon detectors and modulators. The cryogenic operation of a superconducting single photon detector dictates the optimisation of the electro-optic modulators under the same operating conditions. To that end, we characterise a phase modulator, directional coupler, and polarisation converter at both ambient and cryogenic temperatures. The operation voltage of these modulators increases, due to the decrease in the electro-optic effect, by 74% for the phase modulator, 84% for the directional coupler and 35% for the polarisation converter below 8.5. The phase modulator preserves its broadband nature and modulates light in the characterised wavelength range. The unbiased bar state of the directional coupler changed by a wavelength shift of 85 while cooling the device down to 5. The polarisation converter uses periodic poling to phasematch the two orthogonal polarisations. The phasematched wavelength of the utilised poling changes by 112 when cooling to 5.

Enhancement of Birefringence in Borophosphate Pushing Phase-Matching into the Short-Wavelength Region.

Borophosphates are very known for the short ultraviolet (UV) cutoff edge and have become the promising UV and deep-UV functional crystals candidates; however, tetrahedral [PO4] and [BO4] groups own weak anisotropy of polarizability and are not conducive to large birefringence, which hinders their application in the short-wavelength region. Improving their birefringence without compromising the band gap is the main research objective. By introducing the excellent birefringent functional groups, such as [B2O5], [BO2]∞ chain, [B2Ox(OH)5-x], and so forth into borophosphates, seven borophosphates with improved birefringence were successfully synthesized (Δn > 0.05@532 nm). Remarkably, among them, the centimeter-sized crystal of Rb3B8PO16 with a short deep-UV cutoff edge (175 nm) and large birefringence (Δn(exp.) ∼ 0.072@589.3 nm) exhibits the shortest phase-matching wavelength (222 nm), which makes Rb3B8PO16 a promising UV NLO crystal, while KB6PO10(OH)4 with deep-UV cutoff edge features the largest birefringence (Δn(exp.) ∼ 0.103@546 nm) in the reported borophosphate system, making KB6PO10(OH)4 a promising deep-UV birefringent crystal. This study not only provides feasible strategies for increasing the birefringence of borophosphates but also pushes phase-matching into the short-wavelength region.

Highly tunable birefringent phase-matched second-harmonic generation in an angle-cut lithium niobate-on-insulator ridge waveguide.

Phase-matched nonlinear wave mixing, e.g., second-harmonic generation (SHG), is crucial for frequency conversion for integrated photonics and applications, where phase matching wavelength tunability in a wide manner is important. Here, we propose and demonstrate a novel design of angle-cut ridge waveguides for SHG on the lithium niobate-on-insulator (LNOI) platform via type-I birefringent phase matching (BPM). The unique strong birefringence of LN is used to achieve flexible temperature tuning. We experimentally demonstrate a normalized BPM conversion efficiency of 2.7%W-1cm-2 in an angle-cut LN ridge waveguide with a thermo tuning slope of 1.06 nm/K at the telecommunication C band. The approach effectively overcomes the spatial walk-off effect and avoids the need for periodic domain engineering. Furthermore, the angle-cut ridge waveguide scheme can be universally extended to other on-chip birefringent platforms where domain engineering is difficult or immature. The approach may open up an avenue for tunable nonlinear frequency conversion on integrated photonics for broad applications.

Quadratic strong coupling in AlN Kerr cavity solitons.

Photonic platforms with χ(2) nonlinearity offer new degrees of freedom for Kerr frequency comb development. Here, we demonstrate Kerr soliton generation at 1550 nm with phase-matched quadratic coupling to the 775 nm harmonic band in a single AlN microring and thus the formation of dual-band mode-locked combs. In the strong quadratic coupling regime where the χ(2) phase-matching window overlaps the pump mode, the pump-to-harmonic-comb conversion efficiency is optimized. However, the strong quadratic coupling also drastically modifies the Kerr comb generation dynamics and decreases the probability of soliton generation. By engineering the χ(2) phase-matching wavelength, we are able to achieve a balance between high conversion efficiency and high soliton formation rate under the available pump power and microring quality factors. Our numerical simulations confirm the experimental observations. These findings provide guidance on tailoring single-cavity dual-band coherent comb sources.