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RESEARCH PAPER · Angewandte Chemie International Edition · 2024

Enhanced UV Nonlinear Optical Properties in Layered Germanous Phosphites through Functional Group Sequential Construction

Yao Tian, Wei Zeng, Xuehua Dong, Ling Huang, Yuqiao Zhou, Hongmei Zeng, Zhien Lin, Guohong Zou

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Enhanced UV Nonlinear Optical Properties in Layered Germanous Phosphites through Functional Group Sequential ConstructionOriginalFrom Pb6(HPO3)(H2PO3)Cl9 to Pb6(HPO3)2Br8(H2O)·H2O: Halogen Regulation to Achieve Inorganic Metal Phosphite Halide Nonlinear Optical Material with Unprecedented Pb-Centered Polyhedral Units13(C5H12N2S)Hg(NO3)2: A Mercury Nitrate Nonlinear Optical Crystal Motivated by Heteroatom Coordination Strategy9Hydrogen bond-derived symmetry transformation in hydroxyborates: Converting the nonlinearity from null to active7Tetrahedra Modification of Phosphates for Optical Anisotropy Enhancement13Unveiling Noncentrosymmetric Pyridine Carboxylates from Centrosymmetric Templates through Motif Configuration Modulation in Zero-Dimensional System7Two l -Proline Cadmium Thiocyanates with Moderate Second-Harmonic-Generation Responses and Large Birefringences13Novel antimony-based mixed halides exhibiting an excellent SHG response and a broad transmission range20Rational Design and Controlled Synthesis of High-Performance Inorganic Short-Wave UV Nonlinear Optical Materials150Breaking Performance Barriers in KBe 2 BO 3 F 2 (KBBF) Analogs by Functional Group Self‐Polymerization5Breaking Performance Barriers in KBe 2 BO 3 F 2 (KBBF) Analogs by Functional Group Self‐Polymerization48A 3 Sc(PO 4 ) 2 (A = Li, Na): rare earth cations effectively regulate phosphate structures for enhanced birefringence4A remarkable solar-blind ultraviolet nonlinear optical crystal with comprehensive performance and enhanced thermal stability4Bazn2(Hpo3)3: A New Barium Zincophosphite with Short Ultraviolet Cutoff Edge0From NaSc 3 Ga 2 Q 8 (Q = S, Se) to KGa 2 In 3 S 8 : substitution of Sc 3+ with In 3+ to achieve doubled birefringence17From poor-active to high performance via heteroleptic tetrahedra engineering: rational design of non-π-conjugated hybrids for phase-matchable ultraviolet nonlinear optics12Greatly enhancing birefringence of fluorosilicates through the synergetic effect of functional units13Harnessing the dual role of DMSO in the synthesis of SbOCl·DMSO: an excellent nonlinear optical crystal with unique 1D spiral chain10K 2 Na(I 3 O 8 ) 3 : a promising mid-infrared birefringent material with two different structures of octaoxotriiodate( v ) polyanions1Non-centrosymmetric structures designed rationally via a “dimensionality addition” strategy toward the promising nonlinear optical family [A–X][In–Se] (A = K/Ba and Rb/Ba; X = Cl and Br)13Pb 2 B 10 O 16 (OH) 2 ·B(OH) 3 ·H 2 O: significantly enhanced second harmonic generation via substituting metal cations in isostructural compounds with Pb 2+2Significant enhancement in the birefringence of metal phosphite halides via the introduction of π-conjugated cations17Structural chemistry of antimony( iii ) oxalates with lone pairs: polyhedral distortion [SbO 4 F 2 ], π-conjugation [C 2 O 4 ], and birefringence tuning1Synthesising a series of promising ultraviolet nonlinear optical materials with the aid of the flexibility of isolated [B 5 O 10 ] groups3Unprecedented v-shaped [SeO2E] units stabilized in KM[Se2O5]2[SeO2] (M= Al and Ga) constructed by nanoconfinement strategy6Y(C 6 H 5 SO 3 ) 3 ·9H 2 O: strategic integration of ligand substitution and π-conjugated group linkage in sulfates for enhanced ultraviolet nonlinear optical properties4β-LaTeBO 5 and RETeBO 5 (RE = Y, Gd, Tb): explorations of new optical materials in the RE( iii )–Te( iv )–B–O system7Chemical Substitution‐Driven Design of a High‐Performance Noncentrosymmetric Bismuth Molybdenum Selenite10Zwitterionic Glycine-Based Antimony Fluorides with Exceptional Ultraviolet Nonlinear Optical Properties11SnHPO4: A Layered Tin(II) Phosphate with Enhanced Birefringence51Enhanced Birefringence and Excellent Thermal Stability in Two Tellurium(IV) Vanadates: KTeOVO4 and Ca2TeV2O95Regulation of Refractive Index by Halogens in Two-Dimensional Layered Methylsulfonate Halides7A Promising Deep Ultraviolet Nonlinear Optical Crystal Activated by the Ordered Structure Design40A Promising Deep Ultraviolet Nonlinear Optical Crystal Activated by the Ordered Structure Design3Double Sb‐N Coordination Enables Record‐High Birefringence in UV‐Transparent Crystals71Double Sb‐N Coordination Enables Record‐High Birefringence in UV‐Transparent Crystals8Tuning Birefringence in Supramolecular Mg-PDA Frameworks: Modulating Bonding and Layer Connectivity0A new selenide semiconductor NaMn3Ga3Se8 with strong second-harmonic generation and significant luminescence property5Polar [ NH ( CH2SO3 )2]2− Dimers Enable the First Promising Iminodimethanesulfonate with Nonlinear Optical Properties and Wide UV Transparency19Na[B3IO7(OH)] and Na2[B4IO9](IO3): Explorations of Boroiodates with Strong Second Harmonic Generation Response and Large Birefringence54Synthesis, Crystal, and Electronic Structures, and Second Harmonic Generation of La4Ge3S121Sb2(TeO4)(SO4): An Anhydrous Tellurite Sulfate with Large Birefringence and Enhanced Thermal Stability8Halogen-Driven Structural Engineering in Tellurium Oxyhalides: Enhanced SHG Response and Broad Optical Transparency6NH4PO3HCH3 and NH4PO3CH2NH3: Two Phosphate Derivatives with Deep-UV Cutoff Edges and Moderate Birefringence1Chemical Composition Regulation for Tuning the Luminescent Properties of Organic–Inorganic Metal Halides7High Circularly Polarized Luminescence Dissymmetry Factor and Efficient Chiral Second Harmonic Generation in Chiral Hybrid Lead‐Bromide Perovskites13(CH5N3S)2Pb5Br10 and (CH5N3S)Pb2Br4: Two Nonlinear Optical Lead Thiosemicarbazide Bromides with Diverse Pb-Centered Building Units10Assisting the Effective Design of an SBBO-Like Vanadium-Iodate Crystal with Mixed Metal Cations2[CON3H6BF4]: An Efficient Metal‐Free Borate with Optimized Birefringence Achieved by Structural Design Strategy15A Computational Analysis of ZrSe2O6 and HfSe2O6 Oxychalcogenides: Wide-Bandgap Semiconductors with Strain-Tunable Properties0All-three-in-one: Pb2(H2PO4)2(C2O4) significantly enhanced birefringence in phosphate materials4Controllable Synthesis of a Strong Ultraviolet Nonlinear Optical Crystal by Tailoring the Lead Oxychloride Polyhedron3Cation Equivalent Multisubstitution Realizing Structure Transformation and Balanced Nonlinear Optical Performance of Quaternary Eu-Based Chalcogenides8La3Ga5HfO14: Rare-Earth Polyhedron Coupled with Structural Protected Octahedron for Designing Nonlinear Optical Material with Wide Bandgap and Well-Balanced Properties5Non-equivalent terminating roles of hydroxyl and fluorine in hydroxy/fluorooxo-borate optical functional materials2[Ga(C 2 H 6 OS) 6 ](SbBr 6 ): A Highly Luminescent Organic–Inorganic Hybrid Bimetallic Bromide Synthesized via a Cation Hybridization Strategy8(R)‐ and (S)‐SbF3(C8H9NO3): Chiral Antimony‐Based Hybrid Materials with Enhanced Second‐Harmonic Generation and Birefringence4Halide Ion-Directed Symmetry Control in π-Conjugated Molecular Crystals6Designing High-Performance Short-Wave UV Tellurium-Based Mixed Halides Birefringent Crystals via Halogen Substitution Engineering4Y(HPO4)(NO3)(H2O)·2H2O: A Solvent-Responsive Inorganic Layered Material with Reversible Phase Transitions and Optically Active Proton Conductivity2Structures and Nonlinear Optical Properties of Two Acentric Borates with Cubic Cage-like Frameworks5Achieving excellent nonlinear optical performance via “dimensionality elevation”-driven transformation from centrosymmetric to non-centrosymmetric structures1Designing an all-organic wide bandgap ultraviolet nonlinear optical crystal3A balance in SHG response, band gap and birefringence in a series of rare-earth sulfate-iodate6NH4B5O7(OH)2 and CsRbB10O14(OH)4·H2O: Two Hydroxyborates Feature Significant Optical Anisotropy and Contain 1∞[B5O7(OH)2] Chains1Controlling d10 Metal in Phenylthiourea‐Based Hybrid Metal Halides to Actualize Dimensional Transformation and Significantly Improve the Birefringence11A strategy to achieve giant optical anisotropy via integrating linear pseudohalogen and stereochemical active lone pair cation6Hydrogen Bond-Assisted Structural Regulation Enables Large Birefringence in Two Antimony Oxalofluoride Crystals5Achieving large birefringence in oxalate crystals by a hydrogen bond-directed strategy1Hydrogen‐Bond‐Directed Modular Assembly of Polar Chains for Rational Construction of UV Nonlinear Optical Crystals14Hydrogen‐Bond‐Directed Modular Assembly of Polar Chains for Rational Construction of UV Nonlinear Optical Crystals3(CN4H7)H2C3N3S3: Trithiocyanurate Exhibiting Giant Optical Anisotropy via Weak Interaction-Mediated Functional Module Alignment3Anion-Ordered [B3O5(OH)2] Induced by Crystal Water with Deep Ultraviolet Transparency and Large Birefringence in Boron-Rich Borophosphates4From Centrosymmetric Eu 2 Ga 2 S 5 to Noncentrosymmetric EuMg 6 Ga 6 S 16 via Introduction of Distorted MgS 6 Octahedron: Featuring Wide Bandgap and Nonlinear Optical Activity3Synergistic Design of UV Nonlinear Optical Crystals: Harnessing Flexible π-Conjugated Anions and Guanidinium Cations for Enhanced Performance4Recent Progress in the Design and Synthesis of Nonlinear Optical Crystals with Stereochemically Active Lone Pairs8BaZn2(HPO3)3: A New Barium Zincophosphite with Short Ultraviolet Cutoff Edge2K5NaZr4F22(H2O)2: A Hydrated Zirconium Fluoride with a Second-Harmonic Generation Effect and a Short Ultraviolet Cutoff Edge Induced by Cosubstitution with Heterovalent Cations6Enhanced Birefringence in Hybrid Antimony Halides via π-Conjugated Organic Cation Design10Vacancy-driven tetrahedral distortion leading to exceptional second harmonic generation3Research on Nonlinear Optical Materials Based on BO 3 and BO 4 Hydroxy Tetraborates4Organic Halogen Substitution-Driven Halogen Bonding Induces Polar 3D Supramolecular Framework and Second-Harmonic-Generation Response7From (C12H9N2)2TeBr6·2H2O to (C12H9N2)2TeBr6: Dehydration-Driven Crystal Reorganization for Birefringence Optimization6Na6(SO4)2SiF6: A Stable Sulfate Fluosilicate with Wide Deep-Ultraviolet Transparency Window and Strong Second-Harmonic Generation Response4Exceptional Enhancement of Optical Anisotropy Achieved via the Strategy of Combining Rigid Groups with High Symmetry and π‐Conjugated Organic Groups in Hybrid Fluorides33Effect of Multiple Hydrogen Bonding on the π-Conjugated Groups and Optical Properties in Molecular Crystals5pH‐Regulated Ring‐Opening/Closing Transformation in Polyoxometalates Enables High‐Performance Nonlinear Optical Crystals13Unlocking Strong Second‐Harmonic Generation in Deep‐UV‐Transparent Polar Organic Sulfonates through Connectivity Regulation6Stepwise Substitution Strategy for Beryllium-Based Selenites with Enhanced SHG Response, Moderate Birefringence, and Short UV Cutoff Edges6Hybrid Zinc‒Based Halides with Giant Optical Anisotropy via Protonation‒Engineered π ‒Conjugated Organic Group24A Deep-Ultraviolet Transparent Nonlinear Optical Hydrogen-Bonded Organic Framework21A universal synthetic strategy for noncentrosymmetric lead oxyhalide frameworks with strong second-harmonic generation0Polymerization-enhanced optical anisotropy in selenites: a trimeric [H 2 Se 3 O 7 ] motif delivering large UV birefringence0Stable lead succinate-iodides with strong second-harmonic generation response and large birefringence0Strategic Oxygen‐Substitution in Perfluorinated Ce(IV) Coordination Frameworks Triggers Dual‐Wavelength Nonlinear Optical Materials With Exceptional Performances32(C 6 H 7 N 2 O)NO 3 : π-Conjugation-Driven Synergistic Enhancement of Second-Harmonic Generation and Birefringence0Sn 4+ /Sn 2+ Aliovalent Substitution: A Strategy for Local Structure Engineering to Enhance Birefringence and Trigger Structural Symmetry Transition0[C 3 N 2 H 5 ]B 7 O 10 F 2 : Demonstrating a New Hydrogen‐Bond‐Induced Intralayer Charge‐Balanced Structure Model with Large Birefringence3Record‐Short Phase Matchability of Silicate: Charge‐Driven Lattice Distortion Enables Deep‐UV Phase Matching and Strong Optical Nonlinearity0V-Shaped Pseudo-Chains Coupled with Lone-Pair-Distorted [GeX 3 ] − Units Enable Large Birefringence in Ge(II) Hybrid Halides2Helical Mn(II)-based enantiomers based on lactic derivatives with ferroelectric and nonlinear optical properties3Strong Optical Nonlinearity in Polar Hypophosphites via Chiral Cation Assembly1Ultrawide Bandgap and Record-High Birefringence in a Covalent Beryllium-Organic Framework7Enhanced Birefringence in Organic–Inorganic Hybrid Antimony Halides via Partial Halogen Substitution1(C 2 N 4 H 7 S)(H 2 PO 3 ): Optical Properties Study of a Metal‐Free Amidinothiourea Phosphite0The novel Zn-based ultraviolet birefringent crystals combined both large birefringence and wide bandgap2Halogen-Substitution-Modulated Lone-Pair Orientation in Sb(H 2 PO 2 ) 2 X (X = Cl, F) for Enhanced UV Birefringence1Heterometallic Ge–O–Sn-Bridged Oxychalcogenides Sr3GeSnO4Q3 (Q = S, Se) with Wide Band Gaps and Moderate Infrared Nonlinear Optical Responses0Lateral‐Site Unblocking Enables Bilateral π ‐Chromophore Organization for Giant Birefringence in One‐Dimensional Lead Hybrids0Tailoring a Solar‐Blind Ultraviolet Ferroelectric for Nonlinear Optics Through a Local Symmetry‐Breaking Cascaded Strategy1A Two‐Dimensional Organic Salt With a Deep‐Ultraviolet Cutoff Edge and Strong Second‐Harmonic Generation0The Parallel Coplanar Alignment of Planar Non‐π‐Conjugated [Pb 3 Br 3 ] Rings for a Stable Ultraviolet Nonlinear Optical Crystal0Charge and structural flexibility of tartrate groups enable high-performance ultraviolet nonlinear optical crystals0The Multi‐Scale Paradigm: An Integrated Design Logic for Nonlinear Optical Crystals1A Hydrogen-Bonded Molecular Crystal with Strong Optical Anisotropy and Large Second-Harmonic Generation Response0Mixed‐Valence Engineering in Ge 2+ Chalcogenides: Structural Modulation for Balanced Infrared Nonlinear Optics0Dynamic Phosphate Hydrogen‐Bonded Networks Enable Biomedical‐Ready Stabilization of Black Phosphorus0

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  1. From Pb6(HPO3)(H2PO3)Cl9 to Pb6(HPO3)2Br8(H2O)·H2O: Halogen Regulation to Achieve Inorganic Metal Phosphite Halide Nonlinear Optical Material with Unprecedented Pb-Centered Polyhedral Units

    Inorganic Chemistry · 2024-07-08

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  2. (C5H12N2S)Hg(NO3)2: A Mercury Nitrate Nonlinear Optical Crystal Motivated by Heteroatom Coordination Strategy

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  3. Hydrogen bond-derived symmetry transformation in hydroxyborates: Converting the nonlinearity from null to active

    Materials Today Chemistry · 2024-08-29

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  4. Tetrahedra Modification of Phosphates for Optical Anisotropy Enhancement

    Advanced Optical Materials · 2024-08-29

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  5. Unveiling Noncentrosymmetric Pyridine Carboxylates from Centrosymmetric Templates through Motif Configuration Modulation in Zero-Dimensional System

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  6. Two l -Proline Cadmium Thiocyanates with Moderate Second-Harmonic-Generation Responses and Large Birefringences

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  7. Novel antimony-based mixed halides exhibiting an excellent SHG response and a broad transmission range

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  8. Rational Design and Controlled Synthesis of High-Performance Inorganic Short-Wave UV Nonlinear Optical Materials

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  9. Breaking Performance Barriers in KBe 2 BO 3 F 2 (KBBF) Analogs by Functional Group Self‐Polymerization

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  10. Breaking Performance Barriers in KBe 2 BO 3 F 2 (KBBF) Analogs by Functional Group Self‐Polymerization

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  11. A 3 Sc(PO 4 ) 2 (A = Li, Na): rare earth cations effectively regulate phosphate structures for enhanced birefringence

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  12. A remarkable solar-blind ultraviolet nonlinear optical crystal with comprehensive performance and enhanced thermal stability

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  13. Bazn2(Hpo3)3: A New Barium Zincophosphite with Short Ultraviolet Cutoff Edge

    SSRN Electronic Journal · 2025-01-01

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  14. From NaSc 3 Ga 2 Q 8 (Q = S, Se) to KGa 2 In 3 S 8 : substitution of Sc 3+ with In 3+ to achieve doubled birefringence

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  15. From poor-active to high performance via heteroleptic tetrahedra engineering: rational design of non-π-conjugated hybrids for phase-matchable ultraviolet nonlinear optics

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  16. Greatly enhancing birefringence of fluorosilicates through the synergetic effect of functional units

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  17. Harnessing the dual role of DMSO in the synthesis of SbOCl·DMSO: an excellent nonlinear optical crystal with unique 1D spiral chain

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  18. K 2 Na(I 3 O 8 ) 3 : a promising mid-infrared birefringent material with two different structures of octaoxotriiodate( v ) polyanions

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  19. Non-centrosymmetric structures designed rationally via a “dimensionality addition” strategy toward the promising nonlinear optical family [A–X][In–Se] (A = K/Ba and Rb/Ba; X = Cl and Br)

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  20. Pb 2 B 10 O 16 (OH) 2 ·B(OH) 3 ·H 2 O: significantly enhanced second harmonic generation via substituting metal cations in isostructural compounds with Pb 2+

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  21. Significant enhancement in the birefringence of metal phosphite halides via the introduction of π-conjugated cations

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  22. Structural chemistry of antimony( iii ) oxalates with lone pairs: polyhedral distortion [SbO 4 F 2 ], π-conjugation [C 2 O 4 ], and birefringence tuning

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  23. Synthesising a series of promising ultraviolet nonlinear optical materials with the aid of the flexibility of isolated [B 5 O 10 ] groups

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  24. Unprecedented v-shaped [SeO2E] units stabilized in KM[Se2O5]2[SeO2] (M= Al and Ga) constructed by nanoconfinement strategy

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  25. Y(C 6 H 5 SO 3 ) 3 ·9H 2 O: strategic integration of ligand substitution and π-conjugated group linkage in sulfates for enhanced ultraviolet nonlinear optical properties

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  26. β-LaTeBO 5 and RETeBO 5 (RE = Y, Gd, Tb): explorations of new optical materials in the RE( iii )–Te( iv )–B–O system

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  27. Chemical Substitution‐Driven Design of a High‐Performance Noncentrosymmetric Bismuth Molybdenum Selenite

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  28. Zwitterionic Glycine-Based Antimony Fluorides with Exceptional Ultraviolet Nonlinear Optical Properties

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  29. SnHPO4: A Layered Tin(II) Phosphate with Enhanced Birefringence

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  30. Enhanced Birefringence and Excellent Thermal Stability in Two Tellurium(IV) Vanadates: KTeOVO4 and Ca2TeV2O9

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  31. Regulation of Refractive Index by Halogens in Two-Dimensional Layered Methylsulfonate Halides

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  32. A Promising Deep Ultraviolet Nonlinear Optical Crystal Activated by the Ordered Structure Design

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  33. A Promising Deep Ultraviolet Nonlinear Optical Crystal Activated by the Ordered Structure Design

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  34. Double Sb‐N Coordination Enables Record‐High Birefringence in UV‐Transparent Crystals

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  35. Double Sb‐N Coordination Enables Record‐High Birefringence in UV‐Transparent Crystals

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  36. Tuning Birefringence in Supramolecular Mg-PDA Frameworks: Modulating Bonding and Layer Connectivity

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  37. A new selenide semiconductor NaMn3Ga3Se8 with strong second-harmonic generation and significant luminescence property

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  38. Polar [ NH ( CH2SO3 )2]2− Dimers Enable the First Promising Iminodimethanesulfonate with Nonlinear Optical Properties and Wide UV Transparency

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  39. Na[B3IO7(OH)] and Na2[B4IO9](IO3): Explorations of Boroiodates with Strong Second Harmonic Generation Response and Large Birefringence

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  40. Synthesis, Crystal, and Electronic Structures, and Second Harmonic Generation of La4Ge3S12

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  41. Sb2(TeO4)(SO4): An Anhydrous Tellurite Sulfate with Large Birefringence and Enhanced Thermal Stability

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  42. Halogen-Driven Structural Engineering in Tellurium Oxyhalides: Enhanced SHG Response and Broad Optical Transparency

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    Gen Li, Wei Zeng, Gangji Yi, Xuan Zou, Xize Zhan, Hongmei Zeng, Zhien Lin, Guohong Zou

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  43. NH4PO3HCH3 and NH4PO3CH2NH3: Two Phosphate Derivatives with Deep-UV Cutoff Edges and Moderate Birefringence

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  44. Chemical Composition Regulation for Tuning the Luminescent Properties of Organic–Inorganic Metal Halides

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  45. High Circularly Polarized Luminescence Dissymmetry Factor and Efficient Chiral Second Harmonic Generation in Chiral Hybrid Lead‐Bromide Perovskites

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