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RESEARCH PAPER · Journal of the American Chemical Society · 2023

Stereochemically Active Lone-Pair Containing Metal Substitution in Polar Axis toward a Giant Phase-Matchable Optical Nonlinear Silicate Crystal Li 3 (OH)PbSiO 4

Yuanyu Yang, Yan Xiao, Bingxuan Li, Yi-Gang Chen, Penghui Guo, Bingbing Zhang, Xian‐Ming Zhang

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Stereochemically Active Lone-Pair Containing Metal Substitution in Polar Axis toward a Giant Phase-Matchable Optical Nonlinear Silicate Crystal Li 3 (OH)PbSiO 4OriginalSecondary‐Bond‐Driven Construction of a Polar Material Exhibiting Strong Broad‐Spectrum Second‐Harmonic Generation and Large Birefringence9Secondary‐Bond‐Driven Construction of a Polar Material Exhibiting Strong Broad‐Spectrum Second‐Harmonic Generation and Large Birefringence41A UV non-hydrogen pure selenite nonlinear optical material for achieving balanced properties through framework-optimized structural transformation41Ag 2 [TeO 2 (OH) 4 ]: a nonlinear optical tellurate with balanced comprehensive performance2Crystal clear: unveiling giant birefringence in organic–inorganic cocrystals33N 2 H 4 Zn(HC 3 N 3 O 3 ): exceptionally strong second harmonic generation and ultra-long phosphorescence16Noncentrosymmetric tellurite halides created by a depolymerization strategy: toward strong SHG intensity and wide bandgap16Pb 2 (SeO 3 )(SiF 6 ): the first selenite fluorosilicate with a wide bandgap and large birefringence achieved through perfluorinated group modification45Pb 2 Ga 3 F 6 (SeO 3 ) 2 X 3 ·2H 2 O (X = Cl, Br): two new HTO-type members exhibiting large NLO effects mediated by ionic mixing and substitution strategies10From ZnF2 to ZnF2(H2O)4: Partial Substitution Achieves Structural Transformation and Nonlinear Optical Activity while Keeping Short Ultraviolet Cutoff Edge19Dual-Anion Strategy Induces Dual Enhancement Toward Ultrashort Phase-Matching Wavelength in Deep-UV Transparent d0 Transition Metal Oxyfluorides21From Cd(SCN) 2 (CH 4 N 2 S) 2 to Cd(SCN) 2 (C 4 H 6 N 2 ) 2 : Controlling Sulfur Content in Thiocyanate Systems Significantly Improves the Overall Performance of UV Nonlinear Optical Materials9From Cd(SCN) 2 (CH 4 N 2 S) 2 to Cd(SCN) 2 (C 4 H 6 N 2 ) 2 : Controlling Sulfur Content in Thiocyanate Systems Significantly Improves the Overall Performance of UV Nonlinear Optical Materials50[Na2PbI][Ga7S12]: Combining Diamond-Like Anionic Framework with Polycationic Chain toward Achieving Remarkable Nonlinear Optical Response21Layered (C5H6ON)2[Sb2O(C2O4)3] with a large birefringence derived from the uniform arrangement of π-conjugated units11A congruent-melting rubidium zinc vanadium oxychloride exhibiting strong mid-infrared second-harmonic generation and high laser-induced damage threshold6PbBeB2O5: A High-Performance Ultraviolet Nonlinear-Optical Crystal with Functional [BeB2O8]8– Group3(C4H6N3O)(HSO4): A Cytosinium Bisulfate with Large Birefringence and Moderate Second Harmonic Generation Effect Produced via Combining a Promising Planar Nonlinear Optical-Active Motif with a Tetrahedral Group13La3Ga5M0.5Sn0.5O14, (M = Ge, Si): Design and Synthesis of Two Langasite Nonlinear Optical Materials with Large Second Harmonic Generation and Birefringence Induced by Distorted (Sn/M)O6 Octahedra4A2Cd(PO3)4 (A = K, Rb, Cs): Series of cadmium polyphosphates with infinite 1[(PO3)4]ꝏ chains and deep ultraviolet transparency windows2The synthesis, structures and characterizations of (C5H12NO)4Cd3Cl10·2H2O and (C5H12NO)2BiCl6·H5O2 crystals0Two α‐SiO 2 ‐Related Deep‐Ultraviolet Phase‐Matchable Optical Nonlinear Beryllium Silicate Crystals Na 2 BeSiO 4 and Li 2 BeSiO 4 with Enhanced SHG Effect10Chiral-driven formation of hybrid cyanurates with large birefringence2Cationic Coordination Modification Drives Birefringence and Nonlinear Effect Double Lifting in Sulfate4Deep-ultraviolet nonlinear-optical crystals LiBePO 4 and BeP 2 O 6 synthesized by ionic potential modulation towards uniform arrangement of PO 4 groups5Enhanced second-harmonic generation response in a chiral lead iodide induced by amino acid coordination8Stuffed Tridymites A′A″Ga 4 O 8 (A′ = Ba, Sr, Ca; A″ = Pb): Integrating Stereochemically Active Lone Pairs with A-Site Ordering to Design a Polar Structure Featuring Distinctive Ring Topology3A 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 Ca2TeV2O95(C6H10N2)ZnX4·H2O (X=Cl and Br): Excellent nonlinear optical properties and temperature induced photoluminescence for encryption23Methylhydrazine Lone‐Pair Engineering for Polar Lead‐Free Perovskite Enables Self‐Powered X‐Ray Detection4Engineering an Excellent β ‐BaB 2 O 4 ‐Inspired UV Nonlinear Optical Material Through Secondary Building Unit Substitution21Engineering an Excellent β ‐BaB 2 O 4 ‐Inspired UV Nonlinear Optical Material Through Secondary Building Unit Substitution6(3‐C6H10N2)ZnX4 (X = Cl and Br): Two Excellent UV Nonlinear Optical Crystals Designed by Combination of π‐conjugated and [ZnX4]2− Tetrahedral Units26Designed Metal‐Free Quasi‐1D Crystals with Giant Birefringence8Zero-Dimensional Oxyselenide Ba12[(Ga2OSe5)3(Si2O7)]: Enhanced Optical Anisotropy through Heteroanionic Engineering4From AgHgI(SO4) to AgHg3I3.2Cl1.8(SO4): Symmetry Breaking of the Belousovite‐Type Topology by Mixed Halides to Achieve Strong Nonlinear Optical Effect14Improving the Performance of Birefringent Crystals by Molecular Assembly Strategy in the Solar‐Blind UV Region14(CH5N3S)2Pb5Br10 and (CH5N3S)Pb2Br4: Two Nonlinear Optical Lead Thiosemicarbazide Bromides with Diverse Pb-Centered Building Units10La3Ga5HfO14: Rare-Earth Polyhedron Coupled with Structural Protected Octahedron for Designing Nonlinear Optical Material with Wide Bandgap and Well-Balanced Properties5Nonlinear Optical Series A(VO2)3(SeO3)2 (A = NH4+, K+, and H3O+) with Large Birefringence Derived from High-Anisotropic VO6 Octahedra and SeO3 Pyramids8Recent Progress in the Design and Synthesis of Nonlinear Optical Crystals with Stereochemically Active Lone Pairs8Borosilicates as deep-ultraviolet transparent nonlinear optical crystals: Structural motifs, performance limits and future directions9SrZnSiS4: Shattering the 4.0 eV Threshold toward Dual-Optimized Bandgap and Second-Harmonic Generation5Origin of second harmonic generation in noncentrosymmetric crystal structures containing lone pair electrons5Ag3In3(SeO3)3(SO4)F4: A Sulfate Selenite Nonlinear Optical Material with a Wide Bandgap3Metal Chloride‐Iodate Nonlinear Optical Materials via Direct Chlorination of Centrosymmetric Metal Iodate Crystals0LiBa 2 GaSi 2 O 8 : A Noncentrosymmetric Silicate Exhibiting Wide Transmission Range and Moderate Second Harmonic Generation Response2A multi-scale birefringence modulation strategy in DUV/UV crystals induced by organic cations1Anionic configuration extension induced birefringence enhancement in vanadium iodate oxyfluorides0InO6X (X = Cl, Br): distinct functional motif family for nonlinear optical materials51D Cobalt‐Cytidine Monophosphate Coordination Polymer Exhibiting Efficient Ultraviolet Second‐Harmonic Generation7Record‐Short Phase Matchability of Silicate: Charge‐Driven Lattice Distortion Enables Deep‐UV Phase Matching and Strong Optical Nonlinearity0Dual-ligand modulated Lego-like supracluster assembly of Ti-In-oxo clusters and Ag-P clusters for optical limiting applications0An Ultraviolet Transparent Nonlinear Optical Crystal Assembled from a Polarizable Tetrahedral Unit1High‐Performance Infrared Nonlinear Optical Crystals Discovery Guided by High‐Throughput Computation, Machine Learning, and Experimental Verification6High‐Performance Infrared Nonlinear Optical Crystals Discovery Guided by High‐Throughput Computation, Machine Learning, and Experimental Verification2NaNO 3 [(NH 2 ) 2 SO 2 ] 2 : A Halogen‐Free KBBF‐Type Nitrate Crystal with Record Birefringence for Ultraviolet Applications0K 2 ZrSi 2 O 7 with a Wide Transmission Range and Enhanced Birefringence Induced by the d 0 -TM Zr-Based Units2Anion-Stabilized Incommensurate Modulation Enables Nonlinear Optical Response in Eu2SiO3.89N0.110Advances in metal selenite nonlinear optical materials: halogens directed structure modulation and property optimization0Halogen‐Bond Dimensionality Controls π–π Packing to Unlock Ultrahigh Second‐Harmonic Generation and Giant Birefringence0

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  1. Secondary‐Bond‐Driven Construction of a Polar Material Exhibiting Strong Broad‐Spectrum Second‐Harmonic Generation and Large Birefringence

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  2. Secondary‐Bond‐Driven Construction of a Polar Material Exhibiting Strong Broad‐Spectrum Second‐Harmonic Generation and Large Birefringence

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  3. A UV non-hydrogen pure selenite nonlinear optical material for achieving balanced properties through framework-optimized structural transformation

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  4. Ag 2 [TeO 2 (OH) 4 ]: a nonlinear optical tellurate with balanced comprehensive performance

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  5. Crystal clear: unveiling giant birefringence in organic–inorganic cocrystals

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  6. N 2 H 4 Zn(HC 3 N 3 O 3 ): exceptionally strong second harmonic generation and ultra-long phosphorescence

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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. Pb 2 (SeO 3 )(SiF 6 ): the first selenite fluorosilicate with a wide bandgap and large birefringence achieved through perfluorinated group modification

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  9. Pb 2 Ga 3 F 6 (SeO 3 ) 2 X 3 ·2H 2 O (X = Cl, Br): two new HTO-type members exhibiting large NLO effects mediated by ionic mixing and substitution strategies

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  10. From ZnF2 to ZnF2(H2O)4: Partial Substitution Achieves Structural Transformation and Nonlinear Optical Activity while Keeping Short Ultraviolet Cutoff Edge

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  11. Dual-Anion Strategy Induces Dual Enhancement Toward Ultrashort Phase-Matching Wavelength in Deep-UV Transparent d0 Transition Metal Oxyfluorides

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  12. From Cd(SCN) 2 (CH 4 N 2 S) 2 to Cd(SCN) 2 (C 4 H 6 N 2 ) 2 : Controlling Sulfur Content in Thiocyanate Systems Significantly Improves the Overall Performance of UV Nonlinear Optical Materials

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  14. [Na2PbI][Ga7S12]: Combining Diamond-Like Anionic Framework with Polycationic Chain toward Achieving Remarkable Nonlinear Optical Response

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  15. Layered (C5H6ON)2[Sb2O(C2O4)3] with a large birefringence derived from the uniform arrangement of π-conjugated units

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  16. A congruent-melting rubidium zinc vanadium oxychloride exhibiting strong mid-infrared second-harmonic generation and high laser-induced damage threshold

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

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  18. (C4H6N3O)(HSO4): A Cytosinium Bisulfate with Large Birefringence and Moderate Second Harmonic Generation Effect Produced via Combining a Promising Planar Nonlinear Optical-Active Motif with a Tetrahedral Group

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  19. La3Ga5M0.5Sn0.5O14, (M = Ge, Si): Design and Synthesis of Two Langasite Nonlinear Optical Materials with Large Second Harmonic Generation and Birefringence Induced by Distorted (Sn/M)O6 Octahedra

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  22. Two α‐SiO 2 ‐Related Deep‐Ultraviolet Phase‐Matchable Optical Nonlinear Beryllium Silicate Crystals Na 2 BeSiO 4 and Li 2 BeSiO 4 with Enhanced SHG Effect

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  23. Chiral-driven formation of hybrid cyanurates with large birefringence

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

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  25. Deep-ultraviolet nonlinear-optical crystals LiBePO 4 and BeP 2 O 6 synthesized by ionic potential modulation towards uniform arrangement of PO 4 groups

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  27. Stuffed Tridymites A′A″Ga 4 O 8 (A′ = Ba, Sr, Ca; A″ = Pb): Integrating Stereochemically Active Lone Pairs with A-Site Ordering to Design a Polar Structure Featuring Distinctive Ring Topology

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  28. A Wide Band Gap Germanate with the Largest Second Harmonic Generation Response Created by Hypoxic Strategy

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  29. A Wide Band Gap Germanate with the Largest Second Harmonic Generation Response Created by Hypoxic Strategy

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

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  31. (C6H10N2)ZnX4·H2O (X=Cl and Br): Excellent nonlinear optical properties and temperature induced photoluminescence for encryption

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  32. Methylhydrazine Lone‐Pair Engineering for Polar Lead‐Free Perovskite Enables Self‐Powered X‐Ray Detection

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  35. (3‐C6H10N2)ZnX4 (X = Cl and Br): Two Excellent UV Nonlinear Optical Crystals Designed by Combination of π‐conjugated and [ZnX4]2− Tetrahedral Units

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  38. From AgHgI(SO4) to AgHg3I3.2Cl1.8(SO4): Symmetry Breaking of the Belousovite‐Type Topology by Mixed Halides to Achieve Strong Nonlinear Optical Effect

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  42. Nonlinear Optical Series A(VO2)3(SeO3)2 (A = NH4+, K+, and H3O+) with Large Birefringence Derived from High-Anisotropic VO6 Octahedra and SeO3 Pyramids

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  44. Borosilicates as deep-ultraviolet transparent nonlinear optical crystals: Structural motifs, performance limits and future directions

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  47. Ag3In3(SeO3)3(SO4)F4: A Sulfate Selenite Nonlinear Optical Material with a Wide Bandgap

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  48. Metal Chloride‐Iodate Nonlinear Optical Materials via Direct Chlorination of Centrosymmetric Metal Iodate Crystals

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  49. LiBa 2 GaSi 2 O 8 : A Noncentrosymmetric Silicate Exhibiting Wide Transmission Range and Moderate Second Harmonic Generation Response

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  50. A multi-scale birefringence modulation strategy in DUV/UV crystals induced by organic cations

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