Nonlinear Optical Performance Research Articles

Experimental Demonstration of High-Efficiency Harmonic Generation in Photonic Moiré Superlattice Microcavities.

Integrated photonic microcavities have demonstrated powerful enhancement of nonlinear effects, but they face a challenge in achieving critical coupling for sufficient use of incident pump power. In this work, we first experimentally demonstrate that highly efficient third-harmonic generation (THG) and detectable second-harmonic generation (SHG) can be produced from high-Q photonic moiré superlattice microcavities, where a critical coupling condition can be achieved via selecting a magic angle. Furthermore, at the magic angle of 13.17°, critical coupling is satisfied, resulting in a normalized THG conversion efficiency of 136%/W2 at a relatively low peak pump power of 6.8 MW/cm2, which is 3 orders of magnitude higher than the best results reported previously. Our work shows the power of photonic moiré superlattices in enhancing nonlinear optical performances through flexible and feasible engineering resonant modes, which can be applied in integrated frequency conversion and generation of quantum light sources.

Dynamics of the nonlinear optical second- and third-harmonic generation in quantum well due to hydrostatic pressure and temperature

We studied the effects of hydrostatic pressure and temperature on the second- and third-harmonic generation (SHG and THG) in semi-parabolic GaAs/Al0.3Ga0.7As quantum wells. By solving the Schrödinger equation numerically, we can determine the system's sub-band energy levels and wave functions, and then calculate its optical gain. The numerical simulation results show that both temperature and hydrostatic pressure can effectively improve the nonlinear optical performance of the system. Notably, we explore the mechanisms underlying these interactions. These findings suggest a viable approach to adjust the nonlinear optical performance of GaAs/Al0.3Ga0.7As quantum system through the subtle interaction between hydrostatic pressure, temperature and structural parameters.

Homoatomic Polychalcogenide Nonlinear Optical Anionic Groups with Ultra-Large Optical Anisotropy.

Functional assembly of nonlinear optical (NLO) motifs with a large optical anisotropy is vital to the development of advanced NLO and birefringent materials. In this work, we highlight that, in addition to heteroatomic NLO motifs, homoatomic anionic clusters formed by aggregated anions (S, Se, Te) exhibit diverse chain-, ring-, and cage-like chemical structures as well as one-, two-, and three-dimensional motif alignments. The rich structural chemistry enables homoatomic polychalcogenides (HAPCs) to exhibit asymmetric structural features and anisotropic optical properties, with great potential for NLO and birefringent performance. Focusing on totally 55 binary HAPCs A2Qn (n = 2, 3, 4, 5; A = Na, K, Rb, Cs; Q = S, Se, Te) and their ternary analogues, we employ the state-of-the-art first-principles approach to systematically investigate the modulation evolution of their NLO and birefringent properties. Remarkably, Rb2Te3 and Na2TeSe2 exhibit rarely colossal birefringence (>1.0@10 μm) and NLO effects (>20 × AgGaS2), much larger than conventional NLO chalcogenides. Na2Te3 presents the largest birefringence to date (∼3.48@1, 2.72@2, 2.34@10 μm), indicating the unique structural superiority of HAPC in terms of ultra-large birefringence. By mining the intrinsic mechanism, the HAPC anionic groups are identified as novel mid-infrared NLO "material genes", furnishing unique NLO and birefringent performance for the design of novel optoelectronic materials.

Interface engineering and heterometal doping Cu3Se2/WSe2 for efficient charge transfer and nonlinear optical performance

Integrating interface engineering and precious heterometal doping with semiconductors is a feasible pathway to construct efficient charge transfer and improve the nonlinear optical (NLO) performance of materials. Here, we report a bimetallic selenide type-II heterostructure of Cu3Se2/WSe2 (CWS) with a simple one-step magnetron co-sputtering of Cu and WSe2 targets at low argon flow rates. Se first nucleates and precipitates to form nanospheres at low flow rates. Due to the electronegativity of Cu being greater than that of W and Cu prioritizes attachment to the outside of the Se nanospheres and promotes the formation of the nanorods-grown Cu3Se2. A combined analysis of X-ray photoelectron spectroscopy and X-ray diffraction data was used to investigate the minor shift in the W 4 f/Se 2p ratio revealing that electrons shifted from Cu3Se2 to WSe2. The diffraction peaks of CWS and the valence electronic structure of Cu1+/Cu2+ confirmed the implantation of Cu3Se2 nanorods on WSe2. The NLO properties of CWS composite films were modulated by varying the power of Cu. More importantly, the nonlinear absorption coefficient of the CWS composite films formed after Cu3Se2 promotion is much better than that of other unmodified pure WSe2 films. The photogenerated carrier dynamics of CWS composite films were investigated by femtosecond transient absorption spectroscopy, and density functional theory calculations show that CWS composite films inhibit efficient electron transfer photogenerated carrier complexation. This work proposes a few strategies for designing heterogeneous structures with interface engineering and precious metal doping to promote adjustable electron transfer dynamics and achieve high NLO conversion efficiency.

Investigating the Third‐Order NLO Performance of a Three‐Phase Core‐Shell PANI@MIL‐101(Cr)@CeO2 with Internal and External Synergies

AbstractCombining metal–organic frameworks (MOFs) with other functional materials can effectively improve the third‐order nonlinear optical (NLO) performances of MOFs. In this study, two distinct functional materials are selected and a PANI@MIL‐101(Cr)@CeO2 composite is successfully synthesized. The test results of third‐order NLO indicate that introducing PANI regulates the distribution of π electron clouds within the structure of the composite. Additionally, the core@shell structure formed by PANI@MIL‐101(Cr) and CeO2 promotes charge transfer and improves charge transfer efficiency under the weak heterojunction interaction, thereby enhancing nonlinear absorption and refractive signals. Under the double synergistic action of interior and exterior, a new charge transfer occurs between the components of the composite, resulting in excellent third‐order NLO performances. This study indicates that encapsulating polymer and loading metal oxides can effectively improve the NLO response of MOFs, which offers a new idea for more research on multiphase NLO materials.

Role of donor/acceptor of doping on nonlinear optical properties of CdS nanocomposite decorated by carbon quantum dots and reduced graphene oxide

Cadmium sulfide (CdS), reduced graphene oxide (RGO), carbon quantum dots (CQDs), CQDs/CdS and RGO/CdS nanocomposites have been synthesized. The products have been characterized by FESEM, XRD, UV–visible spectroscopy and diffuse reflectance spectroscopy (DRS). The nonlinear optical (NLO) properties of all products are measured using Z-scan technique at 532 nm wavelength. The results reveal that the formation of structures resulting in dπ–pπ delocalized systems makes the samples a perfect choice for NLO devices. NLO properties of CQDs/CdS is attributed to the charges or energy transfer between CQDs and CdS, in the CQDs/CdS hybrid. Overall, the laser excitation of the small CdS (36 nm) in the RGO/CdS hybrid material promotes electron and/or energy transfer to the RGO component. Therefore, RGO has more effect on NLO properties of CdS than CQDs on CdS nanocomposites. This enhanced electron transfer process leads to improved NLO performances, making the hybrid material a promising candidate for various optoelectronic applications.

Design of Pentanary Mixed-Chalcogenides Ag2In2SiS6-xSex (x = 1, 2) Based on the Bucket Effect: Local Structural Difference and High-Performance Nonlinear-Optical Properties Realized by Partial Congener Substitution.

Noncentrosymmetric chalcogenides are promising candidates for infrared nonlinear-optical (NLO) crystals, and exploring high-performance ones is a hot topic and challengeable. Herein, the combination of AgQ4, InQ4, and SiQ4 (Q = S, Se) units with different S/Se ratios resulted in the discovery of the tetrahedral chalcogenides Ag2In2SiS4Se2 (1) and Ag2In2SiS5Se (2). They both crystallize in the monoclinic Cc space group with different local structures. Co-occupied S/Se sites only exist in 2, and the arrangement of [In2SiQ3] six-membered rings builds different helical chains and 3D [(In2SiQ6)2-]n polyanionic frameworks in 1 and 2. They show balanced NLO performances, including phase-matchable moderate NLO responses (0.7 and 0.5 × AGS) and enhanced laser-induced damage thresholds (4.5 and 5.1 × AGS). Theoretical calculations reveal that their NLO responses are predominantly contributed by the AgQ4 and InQ4 units.

A Role of Biosynthesized Zinc Oxide Nanoparticles (ZnO NPs) for Enhancing Seed Quality: A Review

Abiotic and biotic stresses impact seed growth, resulting in economic losses. Seeds are being subjected to an increasing number of biotic and abiotic stress combinations as a result of global warming and climate change, which has adverse effects on their growth and production. Drought, flood, salinity, heavy mineral contamination, cold, and heat were all found to have a negative impact on seed germination. Because of their massive surface area-to-volume ratio, nanoparticles—microscopic pieces with a nanoscale dimension ranging from 1-100 nm—have exceptional thermal conductivity, catalytic reactivity, nonlinear optical performance, and chemical durability. There are various methods for creating nanoparticles, such as chemical, physical, and biological ones. However, because dangerous chemical compounds are used as reducing agents, the chemical and physical procedures are expensive, complicated, and might be hazardous to the environment. The synthesis of nanoparticles using green approaches may be easily scaled up, and they are also cost-effective. Because of their superior qualities, greenly coordinated nanoparticles are currently preferred over traditionally delivered NPs. Green synthesis approaches are particularly appealing due to their ability to reduce nanoparticle toxicity. The use of vitamins, amino acids, and plant extracts has increased as a result. While dangerous and extremely hazardous substances are used in the chemical and physical processes that may cause environmental issues, capping and reducing agents are essential to the synthesis of nanoparticles. The capping or reducing agent used in physical and chemical processes is expensive. When used as a seed treatment, nanoparticles can enhance germination as well as the length, vigor, viability, and quality of the seedlings. This paper aims to provide an overview and evaluation of zinc oxide nanoparticles (ZnO NPs) as a potential substitute for biosynthesised nanoparticles in seed quality improvement.

Realizing the effect of s-block metals on a charge transfer crystal of indol-2-one for enhanced NLO responses with efficient energetic offsets.

Due to their unique photophysical properties, organic charge transfer crystals are becoming promising materials for next-generation optoelectronic devices. This research paper explores the impact of s-block metals on a charge transfer crystal of indol-2-one for enhanced nonlinear optical (NLO) responses with efficient energetic offsets. The study reveals that alkali metals can enhance NLO performance due to their free electrons. The Perdew-Burke-Ernzerhof functional of DFT with dispersion correction (D3) was used, and the λmax values ranged between 596 and 669nm, with the highest value for dichloromethane (DCM). Leveraging the unique properties of metals allowed for the development of nonlinear optical materials with improved performance and versatility. Softness (σ) values provide insight into electron density changes, with higher values indicating a greater tendency for changes and lower values indicating the opposite. The NLO results for the chromophores MMI1-MMI6 show varying linear polarizability (< α0 >) along with their first (β0) and second (γ0) hyperpolarizabilities. Chromophore MMI4 stands out with the highest NLO performance, having two potassium (K) atoms. Its < α0 > , β0, and γ0 values of 4.19, 7.09, and 17.43 (× 10-24 e.s.u), respectively, indicate a significant enhancement in NLO response compared to the other chromophores. The transitions involving (O20)LP → (C3-N5)π* and (O19)LP → (N12-C13)π* exhibit the highest level of stabilization, followed by (O23)π → (C10-C11)π*, while (C6-N12)π → (C6-C7)π* shows the lowest level of stabilization for chromophore MMI4. The present research work is facile in its nature, and it can be helpful for synthetic scientist to design the new materials for uniting crystal properties with metal doping for efficient NLO devices.

Boosted Second Harmonic Generation of a Chiral Hybrid Lead Halide Resonant to Charge Transfer Exciton from Metal Halide Octahedra to Ligand.

Chiral hybrid organic-inorganic metal halides (HOMHs) offer an ideal platform for the advancement of second-order nonlinear optical (NLO) materials owing to their inherent noncentrosymmetric structures. The enhancement of optical nonlinearity of chiral HOMHs could be achieved by matching the free exciton and/or self-trapped exciton energy levels with desired NLO frequencies. However, the current scarcity of resonance modes and low resonance ratio hamper the further improvements of NLO performance. Herein, we propose a new resonant channel of charge transfer (CT) excited states from metal halide polyhedra to organic ligand to boost the second-order optical nonlinearity of chiral HOMHs. The model lead halide (C7H10N)PbBr3 (C7H10N=1-ethylpyridinium) exhibits a drastically enhanced second harmonic generation in resonance to the deep CT exciton energy, with intensity of up to 111.0 times that of KDP and 10.9 times that of urea. The effective NLO coefficient has been determined to be as high as ~40.2 pm V-1, balanced with a large polarization ratio and high laser damage threshold. This work highlights the contribution of organic ligands in the construction of a resonant channel for enhancing second-order NLO coefficients of metal halides, and thus provides guidelines for designing new chiral HOMHs materials for advanced nonlinear photonic applications.

Boosted Second Harmonic Generation of a Chiral Hybrid Lead Halide Resonant to Charge Transfer Exciton from Metal Halide Octahedra to Ligand

AbstractChiral hybrid organic–inorganic metal halides (HOMHs) offer an ideal platform for the advancement of second‐order nonlinear optical (NLO) materials owing to their inherent noncentrosymmetric structures. The enhancement of optical nonlinearity of chiral HOMHs could be achieved by matching the free exciton and/or self‐trapped exciton energy levels with desired NLO frequencies. However, the current scarcity of resonance modes and low resonance ratio hamper the further improvements of NLO performance. Herein, we propose a new resonant channel of charge transfer (CT) excited states from metal halide polyhedra to organic ligand to boost the second‐order optical nonlinearity of chiral HOMHs. The model lead halide (C7H10N)PbBr3 (C7H10N=1‐ethylpyridinium) exhibits a drastically enhanced second harmonic generation in resonance to the deep CT exciton energy, with intensity of up to 111.0 times that of KDP and 10.9 times that of urea. The effective NLO coefficient has been determined to be as high as ~40.2 pm V−1, balanced with a large polarization ratio and high laser damage threshold. This work highlights the contribution of organic ligands in the construction of a resonant channel for enhancing second‐order NLO coefficients of metal halides, and thus provides guidelines for designing new chiral HOMHs materials for advanced nonlinear photonic applications.

Substrate Engineering toward Selective Growth of Ultrathin WC Crystals and Heterostructures via Liquid Cu‐Zn Catalyst

AbstractTransition metal carbides (TMCs) grown by chemical vapor deposition (CVD) offer promise for numerous novel phenomena and applications in the 2D limit. Despite considerable efforts thus far, the flexible customization of TMCs and their heterostructures still remains challenging. Herein, a substrate engineering is developed to achieve customized manufacturing of ultrathin WC single crystals and WC/graphene (WC‐G) heterostructures by varying the concentration of Zn in Cu‐Zn alloy substrate. It is worth noting that Zn atoms can remarkably reduce the nucleation density of graphene and promote the nucleation of WC. Thus, an increasing Zn content is applied to synergistically modulate the growth of graphene and WC, enabling the controllable fabrication of WC and WC‐G heterostructures. The synthesized WC crystals exhibit an ultrathin nature down to 3 nm, as well as high crystalline, ultra‐clean surface, and superb chemical stability. Based on that, the typical metallic properties with a temperature‐dependent resistance (nearly 1.30 Ω at 300 K and nearly 0.08 Ω at 1.7 K) and low resistance as well as excellent nonlinear optical performance of WC are demonstrated. This work provides fresh insights into regulating the growth behavior of multiblock‐structured carbides and promotes the study of their optic and electronic properties.

Perfect Polar Alignment of Parallel Beloamphiphile Layers: Improved Structural Design Bias Realized in Ferroelectric Crystals of the Novel "Methoxyphenyl Series of Acetophenone Azines".

An improved design is described for ferroelectric crystals and implemented with the "methoxyphenyl series" of acetophenone azines, (MeO-Ph, Y)-azines with Y=F (1), Cl (2), Br (3), or I (4). The crystal structures of these azines exhibit polar stacking of parallel beloamphiphile monolayers (PBAMs). Azines 1, 3, and 4 form true racemates whereas chloroazine 2 crystallizes as a kryptoracemate. Azines 1-4 are helical because of the N-N bond conformation. In true racemates the molecules of opposite helicity (M and P) are enantiomers A(M) and A*(P) while in kryptoracemates they are diastereomers A(M) and B*(P). The stacking mode of PBAMs is influenced by halogen bonding, with 2-4 showcasing a kink due to directional interlayer halogen bonding, whereas fluoroazine 1 demonstrates ideal polar stacking by avoiding it. Notably, (MeO-Ph, Y)-azines display a stronger bias for dipole parallel alignment, attributed to the linearity of the biphenyl moiety as compared to the phenoxy series of (PhO, Y)-azines with their non-linear Ph-O-Ph moiety. The crystals of 1-4 all feature planar biphenyls and this synthon facilitates their crystallization through potent triple T-contacts and enhances their nonlinear optical (NLO) performance by increasing conjugation length and affecting favorable chromophore conformations in the solids.

Design and synthesis of a new family of the decanuclear Mn−Ln clusters: A novel approach to nonlinear optical molecular functional materials

For the first time, the {Mn5Ln5} (Ln = Sm (1), Eu (2), Gd (3), Dy (4) and Tb (5)) clusters were synthesized via a one-pot approach utilizing 2-amino-2-methyl-1.3-propanediol as the ligand. The clusters were well-characterized with Single-crystal X-ray diffraction, Powder X-ray diffraction and Fourier Transform Infrared spectra. Magnetic measurements revealed that the compounds 3 and 4 show weak ferromagnetic interactions. Besides, the {Mn5Sm5} film display prominent nonlinear optical performances with the large β of 1.28 × 10−7 m W−1, which indicates a great potential in optical limiting applications. Thus, the discovery of {Mn5Ln5} should open up new avenues for the design of NLO molecular functional materials by using 3 d and/or 4f metal cations.

Controllable Modulation of Third‐Order NLO Properties by Polymer‐Modified MOFs Core@Shell Nanoarchitecture

AbstractThe delocalization and rearrangement of π electron clouds in space is the crucial source of regulating nonlinear optical (NLO) performance. Herein, a core‐shell metal organic framework (MOF)‐heterojunction is constructed to achieve the effect of tuning NLO properties by promoting charge transfer through multiple interactions between heterogeneous interfaces. [Cd(L)(4,4′‐bpy)(H2O)]n (Cd‐MOF) is selected to coat on polyaniline (PANI) surface to form PANI@Cd‐MOF. The constructed heterojunction displays an enhanced reverse saturation absorption (RSA) signal compared with Cd‐MOF, and it should be noted that the third‐order NLO refractive behavior changes from the self‐defocusing of Cd‐MOF to the self‐focusing of PANI@Cd‐MOF. It is proposed that high‐speed electronic communication bridges established via the rich hydrogen bond network (O… H‐N) and π–π interactions between heterogeneous interfaces can effectively modify the π electron cloud density that finally regulates the NLO properties. This work is believed to provide new avenues and insights for the design of third‐order NLO materials.

Novel structure and excellent nonlinear optical performance nanocomposite derived from flower-like MOF grown on MoS2

Molybdenum disulfide (MoS2) is a nonlinear optical material with graphene-like structure. In order to further improve the nonlinear optical performance of MoS2 and expand the application fields of MoS2, we report a simple in-situ self-growth method to functionalize MoS2 nanosheets with metal-organic framework (MOF) for the first time to pursuit excellent reverse saturable absorption performance and optical limiting performance. Firstly, defective MoS2 nanosheets was obtained by chemical etching with H2O2 and cysteamine was inserted into the sulfur vacancies under ultrasound to obtain MoS2–NH2. Then 5,10,15,20-Tetra (4-carbomethoxyphenyl) porphyrin (TCPP) as MOF active growth sites were grafted on MoS2–NH2 by amido linkage to obtain MoS2-TCPP in mild conditions. Finally, flower-like porphyrin-based CuMOF was grown on MoS2-TCPP by solvothermal method to obtain MoS2-CuMOF with stable structure. The third order nonlinear optical performance of MoS2-CuMOF were studied by Z-scan technique. It was found that the third order nonlinear absorption coefficient of MoS2-CuMOF was significantly improved compared with MoS2. Under the same energy of laser irradiation, the third order nonlinear absorption coefficient of MoS2-CuMOF nanocomposite in solution was 6 × 10−10 m/W about 2.3 times of the pristine MoS2 (2.6 × 10−10 m/W). After blending the above materials with polymethyl methacrylate (PMMA) to prepare a solid device, the third order nonlinear absorption coefficient of MoS2-CuMOF/PMMA was 18 × 10−10 m/W about 3.6 times of the MoS2/PMMA (5 × 10−10 m/W). And MoS2-CuMOF/PMMA had better optical limiting ability than MoS2/PMMA. The significant improvement in the performance of the composites can be attributed to the energy transfer between MoS2 and CuMOF, and porphyrin aggregation was inhibited by PMMA after the preparation of devices. Energy transfer can be proved by fluorescence spectroscopy. This work not only provided an example for the covalent functionalization of MoS2, but also offered a new method for designing materials with excellent nonlinear optical performance.

Covalently bonded fluorine optimizing deep-ultraviolet nonlinear optical performance of fluorooxoborates

Covalently bonded fluorine optimizing deep-ultraviolet nonlinear optical performance of fluorooxoborates

Supramolecular Metal Halide Complexes for High-Temperature Nonlinear Optical Switches.

Nonlinear optical (NLO) switching materials, which exhibit reversible intensity modulation in response to thermal stimuli, have found extensive applications across diverse fields including sensing, photoelectronics, and photonic applications. While significant progress has been made in solid-state NLO switching materials, these materials typically showcase their highest NLO performance near room temperature. However, this performance drastically deteriorates upon heating, primarily due to the phase transition undergone by the materials from noncentrosymmetric to centrosymmetric phase. Here, we introduce a new class of NLO switching materials, solid-state supramolecular compounds 18-Crown-6 ether@Cu2Cl4·4H2O (1·4H2O), exhibiting reversible and stable NLO switching when subjected to near-infrared (NIR) photoexcitation and/or thermal stimuli. The reversible crystal structure in response to external stimuli is attributed to the presence of a weakly coordinated bridging water molecule facilitated by hydrogen bonding/chelation interactions between the metal halide and crown-ether supramolecules. We observed an exceptionally high second-harmonic generation (SHG) signal under continuous photoexcitation, even at temperatures exceeding 110 °C. In addition, the bridging water molecules within the complex can be released and recaptured in a fully reversible manner, all without requiring excessive energy input. This feature allows for precise control of SHG signal activation and deactivation through structural transformations, resulting in a high-contrast off/on ratio, reaching values in the million-fold range.

Impact of π-spacer on dye-sensitized solar cells and non-linear optical performance: Styryl vs imine vs azo

Julolidine-based dyes, having a benzoic acid anchoring group, conjugated through different π-bridges (styryl, imine, and azo) have been investigated. It is discovered that the charge transfer (CT) characteristics of the dye system are changed as the π-bridges become less symmetrical. According to TD-DFT studies, the vertical absorption maximum shifts to the red region when the “N” atom is added to the styryl backbone. Computed photovoltaic characteristics, however, indicate that these dyes perform poorly when the “N” atom is added to the styryl backbone. Studies on dye@TiO2 clusters showa possible bonding between these dyes and TiO2, which would cause dye@TiO2 cluster absorption to shift red. Conversely, computed results of linear and non-linear optical (NLO) properties exhibit opposite patterns to those observed in dye-sensitized solar cell (DSSC) performance.Julolidine-based dyes with imine and azo linkers combined with benzoic acid were created and evaluated as DSSC sensitizers to determine their practical application. In agreement with DFT findings, experimental absorption in dimethylformamide (DMF) and cyclic voltammetry (CV) study verified the essential need for HOMO and LUMO energy levels. High thermal stability is indicated by the thermogravimetric analysis (TGA) results, which supports practical applications in DSSCs and non-linear optics (NLO). The efficiency patterns of the fabricated DSSC cells were similar, with JNNC showing the lowest efficiency (0.07 ± 0.02) and JCNC-OH demonstrating the highest (1.94 ± 0.02).

Unearthing Superior Inorganic UV Second-Order Nonlinear Optical Materials: A Mineral-Inspired Method Integrating First-Principles High-Throughput Screening and Crystal Engineering.

Natural minerals, with their adaptable framework structures exemplified by perovskite and lyonsite, have sparked substantial interest as potential templates for the design of advanced functional solid-state materials. Nonetheless, the quest for new materials with desired properties remains a substantial challenge, primarily due to the scarcity of effective and practical synthetic approaches. In this study, we have harnessed a synergistic approach that seamlessly integrates first-principles high-throughput screening and crystal engineering to reinvigorate the often-overlooked fresnoite mineral, Ba2 TiOSi2 O7 . This innovative strategy has culminated in the successful synthesis of two superior inorganic UV nonlinear optical materials, namely Rb2 TeOP2 O7 and Rb2 SbFP2 O7 . Notably, Rb2 SbFP2 O7 demonstrates a comprehensive enhancement in nonlinear optical performance, featuring a shortened UV absorption edge (260 nm) and a more robust second-harmonic generation response (5.1×KDP). Particularly striking is its significantly increased birefringence (0.15@546 nm), which is approximately 30 times higher than the prototype Ba2 TiOSi2 O7 (0.005@546 nm). Our research has not only revitalized the potential of the fresnoite mineral for the development of new high-performance UV nonlinear optical materials but has also provided a clearly defined roadmap for the efficient exploration of novel structure-driven functional materials with targeted properties.