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RESEARCH PAPER · Angewandte Chemie International Edition · 2024

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

Xuehua Dong, Hongbo Huang, Ling Huang, Yuqiao Zhou, Bingbing Zhang, Hongmei Zeng, Zhien Lin, Guohong Zou

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Unearthing Superior Inorganic UV Second‐Order Nonlinear Optical Materials: A Mineral‐Inspired Method Integrating First‐Principles High‐Throughput Screening and Crystal EngineeringOriginal[(C 5 H 6 N 2 ) 2 H](Sb 4 F 13 ): a polyfluoroantimonite with a strong second harmonic generation effect60Design of alkali lead oxybromides with a strong second-harmonic generation response and large birefringence1Designing excellent UV birefringent materials through the synergistic interaction of two highly distorted functional groups23Fully tricoordinated assembly unveils a pioneering nonlinear optical crystal (SbTeO 3 )(NO 3 )25Hydrogen bonding bolstered head-to-tail ligation of functional chromophores in a 0D SbF 3 ·glycine adduct for a short-wave ultraviolet nonlinear optical material32Large optical anisotropy in noncentrosymmetric phosphate with pseudo 2D intercalated layer16Noncentrosymmetric tellurite halides created by a depolymerization strategy: toward strong SHG intensity and wide bandgap16RbSb(SO 4 )(H 2 PO 2 )F: a short-wave UV antimony( iii ) oxysalt with mixed-anions demonstrating enhanced birefringence11Synergistic combination of different types of functional motif in Rb(NO 3 )(SO 3 NH 3 ) for realizing excellent ultraviolet optical nonlinearity18β -CsHg 2 I 5 , a compound with rare [Hg 2 I 5 ] dimers and large optical anisotropy2Hg4(Te2O5)(SO4): A Giant Birefringent Sulfate Crystal Triggered by a Highly Selective Cation153PbBeB2O5: A High-Performance Ultraviolet Nonlinear-Optical Crystal with Functional [BeB2O8]8– Group3Two Short-Wave UV Beryllium Selenites Exhibiting Diverse Optical Properties Stemming from Functional Group Arrangements8Sb2O2SeO3 and Sb2O(SeO3)2: Two-Layered Antimony(III) Selenites with Enhanced Birefringence10Enhanced UV Nonlinear Optical Properties in Layered Germanous Phosphites through Functional Group Sequential Construction11Enhanced UV Nonlinear Optical Properties in Layered Germanous Phosphites through Functional Group Sequential Construction116Old tree blossoms anew: Research progress on the structures and optical properties of ultraviolet selenites56Breaking Boundaries: Giant Ultraviolet Birefringence in Dimension‐Reduced Zn‐Based Crystals66Breaking Boundaries: Giant Ultraviolet Birefringence in Dimension‐Reduced Zn‐Based Crystals8Gradual Increase in Birefringence of Antimony Oxalates through Precise Tuning of the Sb3+/[C2O4]2– Ratio7A3Sc(SO4)3 (A = K, Rb, Cs): Three Deep‐Ultraviolet Transparent Alkali‐Scandium Sulfates with Strong Second‐Harmonic Generation Response and High Thermal Stability14Optimization of Functional Building Blocks Generates a Substantial Improvement in Birefringence from Sn2OSO4 to Sn3O2(OH)(HSO4)6Lanthanide Contraction Eliminates Disorder while Holding Robust Second Harmonic Generation in a Series of Polyiodates13Toward Strong UV–Vis–NIR Second-Harmonic Generation by Dimensionality Engineering of Zinc Thiocyanates32A Giant Optically Anisotropic Phosphate Driven by Mixed Valence Mercury Units22Computer‐Aided Development of New Nonlinear Optical Materials38Computer‐Aided Development of New Nonlinear Optical Materials14Novel 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 Materials150Rapidly Generated, Ultra‐Stable, and Switchable Photoinduced Radicals: A Solid‐State Photochromic Paradigm for Reusable Paper Light‐Writing35Rapidly Generated, Ultra‐Stable, and Switchable Photoinduced Radicals: A Solid‐State Photochromic Paradigm for Reusable Paper Light‐Writing2Cationic Coordination Modification Drives Birefringence and Nonlinear Effect Double Lifting in Sulfate41D Bi ribbon/[PO 4 ] synergy-driven bismuth phosphates for ultraviolet nonlinear optical crystals with large SHG and birefringence0A wide band gap selenohalide Cs 9 Si 8 Se 20 Cl with unprecedented [CsSe 7 Cl] mixed anionic units2Different p-block elements induce C 3 [111] octahedral distortion in titanium to generate an intense nonlinear effect14Exploring new horizons in mid-to-far infrared nonlinear optical crystals: the significant potential of trigonal pyramidal [TeS 3 ] 2− functional units18Harnessing the dual role of DMSO in the synthesis of SbOCl·DMSO: an excellent nonlinear optical crystal with unique 1D spiral chain10Hg 2 (HTe 2 O 5 )(PO 4 ): a novel phosphate crystal with enhanced birefringence enabled by the synergistic modification of multiple functional groups12Y(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 properties4Chemical 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 Birefringence51Dual Lone Pair Strategy for High Birefringence in Antimony(III)-Based Tellurite Sulfates with Short-Wave UV Transparency10New Ways to Discover Novel Nonlinear Optical Materials: Scaling Machine Learning with Chemical Descriptors Information20A Wide Band Gap Germanate with the Largest Second Harmonic Generation Response Created by Hypoxic Strategy22A Wide Band Gap Germanate with the Largest Second Harmonic Generation Response Created by Hypoxic Strategy5Enhanced Birefringence and Excellent Thermal Stability in Two Tellurium(IV) Vanadates: KTeOVO4 and Ca2TeV2O95Size effect of cations in the A2B3O4F3 family: Based on the new member Cs2B3O4F34(C6H10N2)ZnX4·H2O (X=Cl and Br): Excellent nonlinear optical properties and temperature induced photoluminescence for encryption23Double Sb‐N Coordination Enables Record‐High Birefringence in UV‐Transparent Crystals71Double Sb‐N Coordination Enables Record‐High Birefringence in UV‐Transparent Crystals8Expanding the Spectral Range in T2‐Supertetrahedral Nonlinear Optical Chalcogenides via Incorporating Inorganic Polycations4Expanding the Spectral Range in T2‐Supertetrahedral Nonlinear Optical Chalcogenides via Incorporating Inorganic Polycations29A new selenide semiconductor NaMn3Ga3Se8 with strong second-harmonic generation and significant luminescence property5Synergically Assembling Advantageous Groups toward High‐Performance Infrared Nonlinear Optical Materials A II CdSiSe 4 (A II = Sr, Ba)40Polar [ NH ( CH2SO3 )2]2− Dimers Enable the First Promising Iminodimethanesulfonate with Nonlinear Optical Properties and Wide UV Transparency19Potassium Tetraiodatoiodate(III) Iodate(V): A Nonlinear Optical Crystal with Exceptional Second‐Harmonic Generation and Full‐Wavelength Phase Matching19Potassium Tetraiodatoiodate(III) Iodate(V): A Nonlinear Optical Crystal with Exceptional Second‐Harmonic Generation and Full‐Wavelength Phase Matching0Synthesis, Crystal, and Electronic Structures, and Second Harmonic Generation of La4Ge3S121Halogen-Driven Structural Engineering in Tellurium Oxyhalides: Enhanced SHG Response and Broad Optical Transparency6Bridging the Interlayer Binding to Ordered π‐Conjugated Units for Constructing High‐Performing Light Polarization Crystals8Bridging the Interlayer Binding to Ordered π‐Conjugated Units for Constructing High‐Performing Light Polarization Crystals48Synergistic Machine Learning Guided Discovery of ABa 3 (BSe 3 ) 2 X (A = Rb, Cs; X = Cl, Br, I): A Promising Family as Property‐Balanced IR Functional Materials10Chemical Composition Regulation for Tuning the Luminescent Properties of Organic–Inorganic Metal Halides7Methyl substitution induced noncentrosymmetric alignment: a new thiazolium-based nonlinear optical crystal of HDT-N1S2Halide Ion-Directed Symmetry Control in π-Conjugated Molecular Crystals6Dual Chemical Scissors Strategy Enables 1D Antimony Selenates with Ultraviolet Nonlinear Optical Properties35Dual Chemical Scissors Strategy Enables 1D Antimony Selenates with Ultraviolet Nonlinear Optical Properties6Designing High-Performance Short-Wave UV Tellurium-Based Mixed Halides Birefringent Crystals via Halogen Substitution Engineering4Achieving excellent nonlinear optical performance via “dimensionality elevation”-driven transformation from centrosymmetric to non-centrosymmetric structures1Designing an all-organic wide bandgap ultraviolet nonlinear optical crystal3Hydrogen Bond-Assisted Structural Regulation Enables Large Birefringence in Two Antimony Oxalofluoride Crystals5Lewis Acidity‐Governed Ion Exchange and Record Birefringence in A′[Ag 3 (PO 3 F) 2 ]11Lewis Acidity‐Governed Ion Exchange and Record Birefringence in A′[Ag 3 (PO 3 F) 2 ]2Correlation of Energy-Band Structure and Slow-Saturable-Absorption Characteristics for 2D or Bulk TeSe24(CN4H7)H2C3N3S3: Trithiocyanurate Exhibiting Giant Optical Anisotropy via Weak Interaction-Mediated Functional Module Alignment3Recent Progress in the Design and Synthesis of Nonlinear Optical Crystals with Stereochemically Active Lone Pairs8Enhanced Birefringence in Hybrid Antimony Halides via π-Conjugated Organic Cation Design10KF·[SO 2 (NH 2 ) 2 ]: the First Deep‐Ultraviolet Transparent Sulfonamide Fluoride Nonlinear Optical Crystal with Novel Cairo Pentagonal Structure13KF·[SO 2 (NH 2 ) 2 ]: the First Deep‐Ultraviolet Transparent Sulfonamide Fluoride Nonlinear Optical Crystal with Novel Cairo Pentagonal Structure5Breaking the Deep‐UV Transparency/Optical Nonlinearity Trade‐Off: Three‐Parameter Optimization in Oxyfluorides by Tailoring d 0 ‐Metal Incorporation10Breaking the Deep‐UV Transparency/Optical Nonlinearity Trade‐Off: Three‐Parameter Optimization in Oxyfluorides by Tailoring d 0 ‐Metal Incorporation4LnEuGa3OS6 (Ln = La, Pr, Nd): three dual rare earth metal-based oxychalcogenides with good IR nonlinear optical performances1From (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 Response4Tunable optical properties and enhanced nonlinear performance of Cr@Cr₂O₃ films via laser power modulation1Stepwise Substitution Strategy for Beryllium-Based Selenites with Enhanced SHG Response, Moderate Birefringence, and Short UV Cutoff Edges6Chiral Lead-Oxyiodide Nonlinear Optical Crystals Constructed on l -Malate Groups5KCd(IO 3 ) 2 Cl: A New UV NLO Crystal with Balanced Optical Properties Engineering via Target‐Driven Multi‐Ion Substitution Strategy7Sb 2 (SeO 3 ) 2 SeO 4 : A Selenite–Selenate Crystal with Balanced Band Gap and Birefringence3A Homoatomic Heteroleptic Coordination Strategy for Exceptional Infrared Linear and Nonlinear Optical Properties in ANb 2 PS 4 (S 2 ) 3 (A = K,Rb,Cs)3A 2 Sb 2 SO 4 F 6 (A = NH 4 + , Na + ): two sulfate fluoride crystals exhibiting enhanced birefringence driven by stereochemically active antimony( iii )1Defect-engineered Cu 2 O/Co x O heterostructures with built-in electric fields for high-current-density alkaline water splitting4Design of benzoxazolium-based nonlinear optical crystals with large second-order harmonic generation responses0From centrosymmetric (C 4 H 8 N 5 )(SbF 4 ) to polar (C 4 H 7 N 4 O)(SbF 4 ): a new UV nonlinear optical material achieved by functional group modulation8LiPb3GeS4Br3：含孤对电子功能化超四面体的红外非线性光学晶体（特邀）0Polymerization-enhanced optical anisotropy in selenites: a trimeric [H 2 Se 3 O 7 ] motif delivering large UV birefringence0Series of phosphate nonlinear optical materials containing active metal ions with short cut-off edges0Stable lead succinate-iodides with strong second-harmonic generation response and large birefringence0Syntheses, structures and optical properties of two new cadmium antimonites: Cs 4 Cd(SbF 5 ) 3 (H 2 O) 2 and Cd[Sb 7 O 10 (OH)](SO 4 )0立体化学活性孤对电子与极性基元协同构筑高性能紫外非线性光学晶体（NH4）2Sb3F9SeO4（特邀）0Confinement-assembled ultraviolet nonlinear optical crystal from pyridine-expanded π-systems with exhibiting strong SHG and birefringence18Strategic 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 Birefringence0V-Shaped Pseudo-Chains Coupled with Lone-Pair-Distorted [GeX 3 ] − Units Enable Large Birefringence in Ge(II) Hybrid Halides2Density-Compensated Polarizability Anisotropy for Record Birefringence in Short-Wavelength Ultraviolet Inorganic Crystals11Enhanced tripling-performance in [C(NH2)3]4P2O7·H2O as UV nonlinear optical material due to π-conjugated cation and hydrogen bonding intervention1Hydrogen-Bond-Directed Assembly of an Intramolecular Charge-Transfer Compound for Second-Order Nonlinear Optics1Dopant-Engineered Downshifting Nanoparticles with Dual NIR-II Fluorescence and Magnetic Resonance Imaging for Diagnosis and Image-Guided Surgery of Breast Cancer1Magnesium Methylphosphonate Ultraviolet Nonlinear Optical Crystal With Ultrawide Bandgap and Strong Second‐Harmonic Generation Response0Electronegativity Adaption Approach for Solar‐Blind UV Birefringent Crystals With Ultrawide Bandgaps2Defect Diamond‐Like d 10 Metal Indium Selenium With Strong Second‐Harmonic Generation and Enhanced Laser‐Induced Damage Threshold2Enhanced Birefringence in Organic–Inorganic Hybrid Antimony Halides via Partial Halogen Substitution1K 2 ZrSi 2 O 7 with a Wide Transmission Range and Enhanced Birefringence Induced by the d 0 -TM Zr-Based Units2Unlocking Nonlinear Optics and Photoluminescence with Simultaneous Enhancement of Bandgap and Birefringence in Hybrid Sb-Based Halides2Halogen-Substitution-Modulated Lone-Pair Orientation in Sb(H 2 PO 2 ) 2 X (X = Cl, F) for Enhanced UV Birefringence1K 3 Yb 2 (BO 3 ) 3 and Rb 3 Yb 2 (BO 3 ) 3 : Two Rare-Earth Borate Ultraviolet Nonlinear Optical Crystals1Lateral‐Site Unblocking Enables Bilateral π ‐Chromophore Organization for Giant Birefringence in One‐Dimensional Lead Hybrids0A Rare-Earth Borophosphate Ultraviolet Nonlinear Optical Crystal Featuring P–O–P Linkages0Generative inverse design of cold metals for low-power electronics0Record Second-Harmonic Generation and Exceptional Optical Anisotropy in High-Symmetry 1D Polar Perovskites1K3Sr3Li2Ga4B6O20F: A Sr2Be2B2O7-Type Ultraviolet Nonlinear Optical Crystal0Charge and structural flexibility of tartrate groups enable high-performance ultraviolet nonlinear optical crystals0MAlB3O6F2 (M = Ca and Pb): Two New Fluoroaluminoborates Featuring π-Conjugated [BO3] and [AlO4F2] Units with Large Birefringence0

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  1. [(C 5 H 6 N 2 ) 2 H](Sb 4 F 13 ): a polyfluoroantimonite with a strong second harmonic generation effect

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  2. Design of alkali lead oxybromides with a strong second-harmonic generation response and large birefringence

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  3. Designing excellent UV birefringent materials through the synergistic interaction of two highly distorted functional groups

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  4. Fully tricoordinated assembly unveils a pioneering nonlinear optical crystal (SbTeO 3 )(NO 3 )

    Chemical Science · 2024-01-01

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  5. Hydrogen bonding bolstered head-to-tail ligation of functional chromophores in a 0D SbF 3 ·glycine adduct for a short-wave ultraviolet nonlinear optical material

    Chemical Science · 2024-01-01

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  6. Large optical anisotropy in noncentrosymmetric phosphate with pseudo 2D intercalated layer

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  7. Noncentrosymmetric tellurite halides created by a depolymerization strategy: toward strong SHG intensity and wide bandgap

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  8. RbSb(SO 4 )(H 2 PO 2 )F: a short-wave UV antimony( iii ) oxysalt with mixed-anions demonstrating enhanced birefringence

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  9. Synergistic combination of different types of functional motif in Rb(NO 3 )(SO 3 NH 3 ) for realizing excellent ultraviolet optical nonlinearity

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  10. β -CsHg 2 I 5 , a compound with rare [Hg 2 I 5 ] dimers and large optical anisotropy

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  11. Hg4(Te2O5)(SO4): A Giant Birefringent Sulfate Crystal Triggered by a Highly Selective Cation

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  12. PbBeB2O5: A High-Performance Ultraviolet Nonlinear-Optical Crystal with Functional [BeB2O8]8– Group

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  13. Two Short-Wave UV Beryllium Selenites Exhibiting Diverse Optical Properties Stemming from Functional Group Arrangements

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  14. Sb2O2SeO3 and Sb2O(SeO3)2: Two-Layered Antimony(III) Selenites with Enhanced Birefringence

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

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

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  17. Old tree blossoms anew: Research progress on the structures and optical properties of ultraviolet selenites

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  18. Breaking Boundaries: Giant Ultraviolet Birefringence in Dimension‐Reduced Zn‐Based Crystals

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  19. Breaking Boundaries: Giant Ultraviolet Birefringence in Dimension‐Reduced Zn‐Based Crystals

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  20. Gradual Increase in Birefringence of Antimony Oxalates through Precise Tuning of the Sb3+/[C2O4]2– Ratio

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  21. A3Sc(SO4)3 (A = K, Rb, Cs): Three Deep‐Ultraviolet Transparent Alkali‐Scandium Sulfates with Strong Second‐Harmonic Generation Response and High Thermal Stability

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  22. Optimization of Functional Building Blocks Generates a Substantial Improvement in Birefringence from Sn2OSO4 to Sn3O2(OH)(HSO4)

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  23. Lanthanide Contraction Eliminates Disorder while Holding Robust Second Harmonic Generation in a Series of Polyiodates

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  24. Toward Strong UV–Vis–NIR Second-Harmonic Generation by Dimensionality Engineering of Zinc Thiocyanates

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  25. A Giant Optically Anisotropic Phosphate Driven by Mixed Valence Mercury Units

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

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

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  32. Cationic Coordination Modification Drives Birefringence and Nonlinear Effect Double Lifting in Sulfate

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  33. 1D Bi ribbon/[PO 4 ] synergy-driven bismuth phosphates for ultraviolet nonlinear optical crystals with large SHG and birefringence

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  34. A wide band gap selenohalide Cs 9 Si 8 Se 20 Cl with unprecedented [CsSe 7 Cl] mixed anionic units

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  35. Different p-block elements induce C 3 [111] octahedral distortion in titanium to generate an intense nonlinear effect

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  36. Exploring new horizons in mid-to-far infrared nonlinear optical crystals: the significant potential of trigonal pyramidal [TeS 3 ] 2− functional units

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  37. 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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  38. Hg 2 (HTe 2 O 5 )(PO 4 ): a novel phosphate crystal with enhanced birefringence enabled by the synergistic modification of multiple functional groups

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

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

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

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    Xinyue Shi, Xueqing Liu, Chunxiao Nie, Yangkai Zhang, Degao Zhong, Bing Teng, Zhoubin Lin, Yisheng Huang, Shijia Sun

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  43. Dual Lone Pair Strategy for High Birefringence in Antimony(III)-Based Tellurite Sulfates with Short-Wave UV Transparency

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