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RESEARCH PAPER · Angewandte Chemie International Edition · 2021

A Congruent‐Melting Mid‐Infrared Nonlinear Optical Vanadate Exhibiting Strong Second‐Harmonic Generation

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A Congruent‐Melting Mid‐Infrared Nonlinear Optical Vanadate Exhibiting Strong Second‐Harmonic GenerationOriginalA Lanthanum Ammonium Sulfate Double Salt with a Strong SHG Response and Wide Deep‐UV Transparency15A Lanthanum Ammonium Sulfate Double Salt with a Strong SHG Response and Wide Deep‐UV Transparency96LiNbTeO5: A High-Performance Multifunctional Crystal Material with a Very Large Second-Harmonic Generation Response and Piezoelectric Coefficient52Nain(C2o4)(Hpo4)(H2o)5: An Ultraviolet Transparent Nonlinear Optical Oxalate-Phosphate with Large Birefringence0Unprecedented mid-infrared nonlinear optical materials achieved by crystal structure engineering, a case study of (KX)P 2 S 6 (X = Sb, Bi, Ba)59Wide bandgaps and strong SHG responses of hetero-oxyfluorides by dual-fluorination-directed bandgap engineering28High‐Performance Sulfate Optical Materials Exhibiting Giant Second Harmonic Generation and Large Birefringence21High‐Performance Sulfate Optical Materials Exhibiting Giant Second Harmonic Generation and Large Birefringence199HgSO4: An excellent mid-infrared sulfate nonlinear optical crystal with wide band gap and strong second harmonic generation response19Ultrawide Bandgap and Outstanding Second‐Harmonic Generation Response by a Fluorine‐Enrichment Strategy at a Transition‐Metal Oxyfluoride Nonlinear Optical Material51Ultrawide Bandgap and Outstanding Second‐Harmonic Generation Response by a Fluorine‐Enrichment Strategy at a Transition‐Metal Oxyfluoride Nonlinear Optical Material12Two Mixed Alkali-Metal Borates Templated from Cations to Clusters10Transparent Lead‐Free Ferroelectric (K, Na)NbO3 Single Crystal with Giant Second Harmonic Generation and Wide Mid‐Infrared Transparency Window21Ternary AGa5S8 (A = K, Rb, Cs): Promising infrared nonlinear optical materials rationally realized by “one-for-multiple substitution” strategy37Large second harmonic generation in a penta-CdO 2 sheet exfoliated from its bulk phase16Ce 3 F 4 (SO 4 ) 4 : cationic framework assembly for designing polar nonlinear optical material through fluorination degree modulation23LiVTeO 5 : a mid-infrared nonlinear optical vanadium tellurate crystal exhibiting enhanced second harmonic generation activities and notable birefringence21The first polyanion-substitution-driven centrosymmetric-to-noncentrosymmetric structural transformation realizing an excellent nonlinear optical supramolecule [Cd 4 P 2 ][CdBr 4 ]17Toward Large Second-Harmonic Generation and Deep-UV Transparency in Strongly Electropositive Transition Metal Sulfates112Optimal Design of Mid-Infrared Nonlinear-Optical Crystals: From SrZnSnSe 4 to SrZnSiSe 422Cd2Nb2Te4O15: A Novel Pseudo‐Aurivillius‐Type Tellurite with Unprecedented Nonlinear Optical Properties and Excellent Stability40Hg3(SeO3)2(SO4): A UV Nonlinear Optical Mercury Selenite Sulfate Constructed by Neat [Hg6O8(SeO3)4]∞ Layers and SO4 Tetrahedra27Quadruple‐Bidentate Nitrate‐Ligated A 2 Hg(NO 3 ) 4 (A=K, Rb): Strong Second‐Harmonic Generation and Sufficient Birefringence59Quadruple‐Bidentate Nitrate‐Ligated A 2 Hg(NO 3 ) 4 (A=K, Rb): Strong Second‐Harmonic Generation and Sufficient Birefringence2From Layered Borate to Porous-Layered Aluminoborate7A potassium lead 2-methylmalonate-iodide nonlinear optical crystal with strong second-harmonic generation response and large birefringence2Ultrashort Phase‐Matching Wavelength and Strong Second‐Harmonic Generation in Deep‐UV‐Transparent Oxyfluorides by Covalency Reduction33Ultrashort Phase‐Matching Wavelength and Strong Second‐Harmonic Generation in Deep‐UV‐Transparent Oxyfluorides by Covalency Reduction3K4ZnV5O15Cl: A Congruent‐Melting Mid‐Infrared Nonlinear Optical Crystal Combined with Strong Second‐Harmonic Generation and High Laser‐Induced Damage Threshold14Secondary‐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 defect pyrochlore-like acentric cubic lead titanium-tellurate crystal exhibiting strong second harmonic generation activity and an extended transparent window4New ultraviolet transparent rare-earth borates with enhanced birefringence induced by cation chemical substitution15Rb 8 Nb 10 Ge 6 O 41 : a new niobium-germanate crystal featuring unique one-dimensional [Nb 7 O 30 ] ∞ chains and wide mid-IR transparency2Three in one: a cadmium bismuth vanadate NLO crystal exhibiting a large second-harmonic generation response and enhanced birefringence12Halogen-assisted octet binding electrons construction of pnictogens towards wide-bandgap nonlinear optical pnictides17Unearthing Superior Inorganic UV Second‐Order Nonlinear Optical Materials: A Mineral‐Inspired Method Integrating First‐Principles High‐Throughput Screening and Crystal Engineering124Unearthing Superior Inorganic UV Second‐Order Nonlinear Optical Materials: A Mineral‐Inspired Method Integrating First‐Principles High‐Throughput Screening and Crystal Engineering4Record Second-Harmonic Generation and Birefringence in an Ultraviolet Antimonate by Bond Engineering157A congruent-melting rubidium zinc vanadium oxychloride exhibiting strong mid-infrared second-harmonic generation and high laser-induced damage threshold6A Rare Earth Chalcogenide Nonlinear Optical Crystal KLaGeS4: Achieving Good Balance among Band Gap, Second Harmonic Generation Effect, and Birefringence12Bridgman growth and characterizations of nonlinear optical crystal La3Ga5.5Nb0.5O140Polar-Layer-Driven Reconstruction of a Noncentrosymmetric Vandate Mid-Infrared Nonlinear-Optical Crystal10Exploring quaternary vanadates containing alkali metals, alkaline earth metals, and [VO 4 ] in the quest for nonlinear optical materials1pH‐Dependent Switching Between Nonlinear‐Optical‐Active Nitrate‐Based Supramolecular Polymorphs27pH‐Dependent Switching Between Nonlinear‐Optical‐Active Nitrate‐Based Supramolecular Polymorphs2Oxygen‐Substitution Induced High‐Performance Nonlinear Optical Properties: Witnessed by the First Quaternary Oxythiostannate12Ca 7 (TeO 3 ) 6 (MoO 4 ): A Promising Mid-Infrared Nonlinear Optical Crystal Activated via a Module-Oriented Dimensionality Reduction Strategy34Cs2CdV2O6Br2: A Mid-Infrared Nonlinear Optical Vanadate Containing Both d0/d10 Transition Metal Cations and Bromine Anions5From Centrosymmetric Ca3Ge2O3S4 to Noncentrosymmetric Ca3Ge2O4Se3: A Nonlinear Optical Ca-Based Oxyselenide5SrZnSiS4: Shattering the 4.0 eV Threshold toward Dual-Optimized Bandgap and Second-Harmonic Generation5SrZnGeSe4: An Infrared Nonlinear Optical Crystal Material with Wide Transmission Range and Large SHG Response6A Band‐Orientation Co‐Anchoring Strategy for the Design of a High‐Performance Mid‐Infrared Nonlinear Optical Crystal12pH‐Regulated Ring‐Opening/Closing Transformation in Polyoxometalates Enables High‐Performance Nonlinear Optical Crystals13Symmetry‐Aware Equivariant Network for Discovering SHG‐Active Materials5Mid Infrared Nonlinear Optical Series A 4 MV 5 O 15 X (A = K, Rb; M = Zn, Cd; X = Cl, Br) with Strong Second Harmonic Generation Responses3Stable lead succinate-iodides with strong second-harmonic generation response and large birefringence0中红外氧化物非线性光学晶体研究进展(特邀)0Rational design of a quasi-0D tungsten tellurite nonlinear optical crystal with exceptionally balanced properties1Heterometallic Ge–O–Sn-Bridged Oxychalcogenides Sr3GeSnO4Q3 (Q = S, Se) with Wide Band Gaps and Moderate Infrared Nonlinear Optical Responses0Non-π-conjugated tetrahedra-based optical crystals: The improvement of the linear and nonlinear optical properties by the combination of trigonal pyramidal [XO3] (X = I, Se, Te) units1Λ‐Shaped Dimers Enables Polar Antiperovskites Through A‐Site Displacement Mechanism0A Telluromolybdate Mid-Infrared Nonlinear Optical Crystal with Wide Transparency and Strong Second-Harmonic Generation Response0

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  2. A Lanthanum Ammonium Sulfate Double Salt with a Strong SHG Response and Wide Deep‐UV Transparency

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  3. LiNbTeO5: A High-Performance Multifunctional Crystal Material with a Very Large Second-Harmonic Generation Response and Piezoelectric Coefficient

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  4. Nain(C2o4)(Hpo4)(H2o)5: An Ultraviolet Transparent Nonlinear Optical Oxalate-Phosphate with Large Birefringence

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  5. Unprecedented mid-infrared nonlinear optical materials achieved by crystal structure engineering, a case study of (KX)P 2 S 6 (X = Sb, Bi, Ba)

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  6. Wide bandgaps and strong SHG responses of hetero-oxyfluorides by dual-fluorination-directed bandgap engineering

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  7. High‐Performance Sulfate Optical Materials Exhibiting Giant Second Harmonic Generation and Large Birefringence

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  8. High‐Performance Sulfate Optical Materials Exhibiting Giant Second Harmonic Generation and Large Birefringence

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  9. HgSO4: An excellent mid-infrared sulfate nonlinear optical crystal with wide band gap and strong second harmonic generation response

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  10. Ultrawide Bandgap and Outstanding Second‐Harmonic Generation Response by a Fluorine‐Enrichment Strategy at a Transition‐Metal Oxyfluoride Nonlinear Optical Material

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  11. Ultrawide Bandgap and Outstanding Second‐Harmonic Generation Response by a Fluorine‐Enrichment Strategy at a Transition‐Metal Oxyfluoride Nonlinear Optical Material

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  12. Two Mixed Alkali-Metal Borates Templated from Cations to Clusters

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  13. Transparent Lead‐Free Ferroelectric (K, Na)NbO3 Single Crystal with Giant Second Harmonic Generation and Wide Mid‐Infrared Transparency Window

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  14. Ternary AGa5S8 (A = K, Rb, Cs): Promising infrared nonlinear optical materials rationally realized by “one-for-multiple substitution” strategy

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  15. Large second harmonic generation in a penta-CdO 2 sheet exfoliated from its bulk phase

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  16. Ce 3 F 4 (SO 4 ) 4 : cationic framework assembly for designing polar nonlinear optical material through fluorination degree modulation

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  17. LiVTeO 5 : a mid-infrared nonlinear optical vanadium tellurate crystal exhibiting enhanced second harmonic generation activities and notable birefringence

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  18. The first polyanion-substitution-driven centrosymmetric-to-noncentrosymmetric structural transformation realizing an excellent nonlinear optical supramolecule [Cd 4 P 2 ][CdBr 4 ]

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  19. Toward Large Second-Harmonic Generation and Deep-UV Transparency in Strongly Electropositive Transition Metal Sulfates

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  20. Optimal Design of Mid-Infrared Nonlinear-Optical Crystals: From SrZnSnSe 4 to SrZnSiSe 4

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  21. Cd2Nb2Te4O15: A Novel Pseudo‐Aurivillius‐Type Tellurite with Unprecedented Nonlinear Optical Properties and Excellent Stability

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  22. Hg3(SeO3)2(SO4): A UV Nonlinear Optical Mercury Selenite Sulfate Constructed by Neat [Hg6O8(SeO3)4]∞ Layers and SO4 Tetrahedra

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  23. Quadruple‐Bidentate Nitrate‐Ligated A 2 Hg(NO 3 ) 4 (A=K, Rb): Strong Second‐Harmonic Generation and Sufficient Birefringence

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  24. Quadruple‐Bidentate Nitrate‐Ligated A 2 Hg(NO 3 ) 4 (A=K, Rb): Strong Second‐Harmonic Generation and Sufficient Birefringence

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  26. A potassium lead 2-methylmalonate-iodide nonlinear optical crystal with strong second-harmonic generation response and large birefringence

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  27. Ultrashort Phase‐Matching Wavelength and Strong Second‐Harmonic Generation in Deep‐UV‐Transparent Oxyfluorides by Covalency Reduction

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  29. K4ZnV5O15Cl: A Congruent‐Melting Mid‐Infrared Nonlinear Optical Crystal Combined with Strong Second‐Harmonic Generation and High Laser‐Induced Damage Threshold

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

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

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  32. A defect pyrochlore-like acentric cubic lead titanium-tellurate crystal exhibiting strong second harmonic generation activity and an extended transparent window

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  33. New ultraviolet transparent rare-earth borates with enhanced birefringence induced by cation chemical substitution

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  34. Rb 8 Nb 10 Ge 6 O 41 : a new niobium-germanate crystal featuring unique one-dimensional [Nb 7 O 30 ] ∞ chains and wide mid-IR transparency

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  36. Halogen-assisted octet binding electrons construction of pnictogens towards wide-bandgap nonlinear optical pnictides

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  42. Bridgman growth and characterizations of nonlinear optical crystal La3Ga5.5Nb0.5O14

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  44. Exploring quaternary vanadates containing alkali metals, alkaline earth metals, and [VO 4 ] in the quest for nonlinear optical materials

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  47. Oxygen‐Substitution Induced High‐Performance Nonlinear Optical Properties: Witnessed by the First Quaternary Oxythiostannate

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  48. Ca 7 (TeO 3 ) 6 (MoO 4 ): A Promising Mid-Infrared Nonlinear Optical Crystal Activated via a Module-Oriented Dimensionality Reduction Strategy

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  49. Cs2CdV2O6Br2: A Mid-Infrared Nonlinear Optical Vanadate Containing Both d0/d10 Transition Metal Cations and Bromine Anions

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  50. From Centrosymmetric Ca3Ge2O3S4 to Noncentrosymmetric Ca3Ge2O4Se3: A Nonlinear Optical Ca-Based Oxyselenide

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