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RESEARCH PAPER · Angewandte Chemie International Edition · 2021

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

Chao Wu, Xingxing Jiang, Yilei Hu, Chunbo Jiang, Tianhui Wu, Zheshuai Lin, Zhipeng Huang, Mark Graeme Humphrey, Chi Zhang

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A Lanthanum Ammonium Sulfate Double Salt with a Strong SHG Response and Wide Deep‐UV TransparencyOriginalCsAB 8 O 12 F 2 ·CsI (A = K + , NH 4 + ): design of two fluorooxoborates with benign layered structures via a salt-inclusion strategy28Halogen regulation triggers structural transformation from centrosymmetric to noncentrosymmetric switches in tin phosphate halides Sn 2 PO 4 X (X = F, Cl)47Nain(C2o4)(Hpo4)(H2o)5: An Ultraviolet Transparent Nonlinear Optical Oxalate-Phosphate with Large Birefringence0Cs2Bi2OSi2O7: A Promising Bismuth Silicate Nonlinear Optical Crystal with Face-Sharing BiO5 Polyhedra Exhibiting Strengthened Second Harmonic Generation Response and Birefringence43Exploration of the Crystal Structure and Thermal and Spectroscopic Properties of Monoclinic Praseodymium Sulfate Pr2(SO4)334[C(NH2)3]2Zn(CO3)2: A Guanidinium-Templated Ultraviolet Nonlinear Optical Material20Local Polarity-Induced Assembly of Second-Order Nonlinear Optical Materials128LiRE(SO 4 ) 2 (RE = Y, Gd, Eu): noncentrosymmetric chiral rare-earth sulfates with very large band gaps21NaHSO4·H2O: A Promising Deep-Ultraviolet Nonlinear-Optical Bisulfate with Large Birefringence and a Second-Harmonic-Generation Effect16A lithium–scandium sulfate with second-harmonic generation response and deep-ultraviolet transparency7Breaking the bottleneck of simultaneously wide band gap and large nonlinear optical coefficient by a “pore reconstruction” strategy in a salt-inclusion chalcogenide26Enhancing birefringence of non-π-conjugated sulfate systems through rare-earth metal-centered polyhedra10Modulating optical performance by phase transition in a nonlinear optical material β-Li 2 RbBi(PO 4 ) 28Tetrahedron-based deep-ultraviolet nonlinear optical crystal with optimized KBe 2 BO 3 F 2 -like structure and disordered cations2Deep Eutectic Solvents Synthesis of A2Sb(C2O4)Cl3 (A = NH4, K, Rb) with Superior Optical Performance26Rational Design of the First Ammonium Magnesium Borate with Deep-Ultraviolet Cutoff Edge and Moderate Birefringence and Further Investigation into the Nature of Ammonium in the Borate System15Two Mixed-Alkali-Metal Selenates as Short-Wave Ultraviolet Nonlinear-Optical Materials10Cs 3 [(BOP) 2 (B 3 O 7 ) 3 ]: A Deep-Ultraviolet Nonlinear Optical Crystal Designed by Optimizing Matching of Cation and Anion Groups169Improved Birefringence Activated by Tetrahedra Decorated with a Single Linear Unit38Improved Birefringence Activated by Tetrahedra Decorated with a Single Linear Unit1From Monofluorophosphates A2PO3F to Difluorophosphates APO2F2 (A = alkali metal): Design of a Potential Deep-Ultraviolet Nonlinear Optical Materials System with a Shortened Phase-Matching Wavelength41The Strategy to Improve the Phase Matching Ability in Tetrahedron‐Based Deep‐Ultraviolet Nonlinear Optical Crystals21Nonlinear optical inorganic sulfates: The improvement of the phase matching ability driven by the structural modulation41Quadruple‐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 Birefringence2A Non‐π‐Conjugated Molecular Crystal with Balanced Second‐Harmonic Generation, Bandgap, and Birefringence10Enlargement of Bandgap and Birefringence in Nonlinear Optical Alkali‐Metal Sulfate Crystals by the Substitution of Asymmetrical Non‐π‐Conjugated Cation8YSO4F·H2O: A Deep-Ultraviolet Birefringent Rare-Earth Sulfate Fluoride with Enhanced Birefringence Induced by Fluorinated Y-Centered Polyhedra19Ultrashort 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 Reduction3A Ferroelectric Nonlinear Optical Crystal for Deep‐UV Quasi‐Phase‐Matching51A2Hgx(SeO3)y (A = K, Rb, Cs): Three Alkali Metal Mercury Selenites Featuring Unique 1D [HgOm(SeO3)n]∞ Chains13Secondary‐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 bifunctional primitive strategy induces enhancements of large second harmonic generation and wide UV transmittance in rare-earth borates containing [B 5 O 10 ] groups22A chiral sodium lanthanum sulfate for second-order nonlinear optics and proton conduction6Large optical anisotropy in noncentrosymmetric phosphate with pseudo 2D intercalated layer16RbSb(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 nonlinearity18Giant Optical Anisotropy in a Covalent Molybdenum Tellurite via Oxyanion Polymerization43Li13YGe4O16: A Mid-infrared Rare-Earth Germanate Nonlinear Optical Crystal Featuring a Broad Transmission Range and an Enlarged Band Gap10Sulfate Doping Promotes Agglomeration of Calcium Fluoride Crystals16Hg4(Te2O5)(SO4): A Giant Birefringent Sulfate Crystal Triggered by a Highly Selective Cation153From 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 Materials50A2Pb3[H2N(CH2COO)2]3Cl5 (A = K, Rb): Porous Crystals Constructed on [Pb3Cl5O6] Clusters with Comprehensive Nonlinear Optical Performance3A Universal Design Strategy Achieving Large Birefringence and Short Phase‐Matching Capability of Optical Materials via Dissimilating Non‐π‐Conjugated Units6PbBeB2O5: A High-Performance Ultraviolet Nonlinear-Optical Crystal with Functional [BeB2O8]8– Group3Enhanced 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 Construction116A3Sc(SO4)3 (A = K, Rb, Cs): Three Deep‐Ultraviolet Transparent Alkali‐Scandium Sulfates with Strong Second‐Harmonic Generation Response and High Thermal Stability14NaK5La2(SO4)6: Enhanced Birefringence of Multiple-Alkali Metal Sulfate Systems via Rare Earth Metal-Centered Polyhedra5Optimization of Functional Building Blocks Generates a Substantial Improvement in Birefringence from Sn2OSO4 to Sn3O2(OH)(HSO4)6Screening Strategy Identifies an Overlooked Deep‐Ultraviolet Transparent Nonlinear Optical Crystal3Screening Strategy Identifies an Overlooked Deep‐Ultraviolet Transparent Nonlinear Optical Crystal45Sulfate Derivatives with Heteroleptic Tetrahedra: New Deep‐Ultraviolet Birefringent Materials in which Weak Interactions Modulate Functional Module Ordering61Sulfate Derivatives with Heteroleptic Tetrahedra: New Deep‐Ultraviolet Birefringent Materials in which Weak Interactions Modulate Functional Module Ordering4K4Cd3Ge4O13: A Congruent-Melting Germanate Nonlinear Optical Crystal with a Moderate Second-Harmonic Generation Intensity and Broad Transparent Window2Li2NaB3S2O12: A Deep-UV Transparent Borosulfate with Moderate Birefringence Derived from the [B3S2O12]∞ Infinite Chain Designed by the High Boron-to-Sulfur Ratio Strategy6Two 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 Effect10Unveiling Noncentrosymmetric Pyridine Carboxylates from Centrosymmetric Templates through Motif Configuration Modulation in Zero-Dimensional System7The New Paradigm of Ligand Substitution-Driven Enhancement of Anisotropy from SO4 Units in Short-Wavelength Region14(CN 4 H 7 ) 2 SO 4 ·H 2 O: high-performance metal-free ultraviolet birefringent crystal with KBBF-like configuration5A strongly birefringent sulfate crystal with a wide second-harmonic generation phase-matching range4An excellent ultraviolet nonlinear optical crystal derived from the polar methylphosphonate unit8Different p-block elements induce C 3 [111] octahedral distortion in titanium to generate an intense nonlinear effect14Multifactorial Directed Regulation Of the [Io 3 ] − Units in Praseodymium-Contained Iodates0Structure modulation by cationic modification of sulfates using planar CS(NH 2 ) 25Polar [ NH ( CH2SO3 )2]2− Dimers Enable the First Promising Iminodimethanesulfonate with Nonlinear Optical Properties and Wide UV Transparency19Sb2(TeO4)(SO4): An Anhydrous Tellurite Sulfate with Large Birefringence and Enhanced Thermal Stability8From AgHgI(SO4) to AgHg3I3.2Cl1.8(SO4): Symmetry Breaking of the Belousovite‐Type Topology by Mixed Halides to Achieve Strong Nonlinear Optical Effect14Designing a 3‐Hydroxypropane‐1‐Sulfonate Deep‐Ultraviolet Nonlinear Optical Crystal9CsLa(SO 4 ) 2 : A Lanthanum Sulfate Crystal for Nonlinear Optical Applications10Enhancement of optical anisotropy from [BF4] units by ligand substitution0A Promising Short-Wave UV NLO Crystal with an Optimized KBBF-like Structure and Well-Balanced Properties Achieved via a Chemical Substitution Strategy6(CN4H7)H2C3N3S3: Trithiocyanurate Exhibiting Giant Optical Anisotropy via Weak Interaction-Mediated Functional Module Alignment3Multifactorial directed regulation of anionic units in praseodymium-contained iodates1From centrosymmetric CN3H6C6H5SO3 to non-centrosymmetric CN3H6C6H4SO3(OH): Hydroxyl introduced hydrogen bond reconstruction to realize strong second harmonic generation3KF·[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 Structure5Na6(SO4)2SiF6: A Stable Sulfate Fluosilicate with Wide Deep-Ultraviolet Transparency Window and Strong Second-Harmonic Generation Response4Ag(Te2O3)(PO4): The first Ag-containing phosphate-tellurite nonlinear optical crystal featuring novel zigzag layered structure0Enhancement of Birefringence in Alkali Metal Sulfates Induced by Rare Earth Metal-Centered Polyhedra and Structure Regulation via Cations2A Deep-Ultraviolet Transparent Nonlinear Optical Hydrogen-Bonded Organic Framework21A[N(SO 2 NH 2 ) 2 ] (A = Na, K, Rb, and Cs): enhancing birefringence of non π-conjugated deep-ultraviolet crystals via novel dimeric disulfonamide [N(SO 2 NH 2 ) 2 ] − groups0RbLa(SO 4 ) 2 : A KBBF-like Deep-UV Transparent Rare Earth Sulfate with Strong SHG Response and High Thermal Stability Enabled by Multicomponent Structural Design2Atom-Response-Theory-Guided Design of Chiral Niobium Halides with both a Large Nonlinear Coefficient and Strong Chiroptical Nonlinearity3Record‐Short Phase Matchability of Silicate: Charge‐Driven Lattice Distortion Enables Deep‐UV Phase Matching and Strong Optical Nonlinearity0An Ultraviolet Transparent Nonlinear Optical Crystal Assembled from a Polarizable Tetrahedral Unit1Dimensionality Engineering of Fluorozirconium Phosphates for Deep-UV-Transparent Crystals with Enhanced Second-Harmonic Generation and Birefringence10(CN 4 H 7 )(NH 2 SO 3 ): A Solar‐Blind Ultraviolet Nonlinear Optical Crystal With Short UV Cutoff Edge and Full‐Wavelength Phase‐Matching0Enhancing Birefringence of Sulphates by Polarity Modification in Planar Cations0K 3 Yb 2 (BO 3 ) 3 and Rb 3 Yb 2 (BO 3 ) 3 : Two Rare-Earth Borate Ultraviolet Nonlinear Optical Crystals1Covalent Interlayer Engineering Enables Ideal Birefringence and Strong SHG in Beryllium‐Free Deep‐UV NLO Borates2Symmetry Breaking Induced by Hydration-Number Tuning Enables Second-Order Nonlinear Optical Responses in Lanthanum Sulfate Hydrates0Two Rare Earth-Based Sulfates with Enhanced Birefringence and Broad Optical Transparency Window0

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  2. Halogen regulation triggers structural transformation from centrosymmetric to noncentrosymmetric switches in tin phosphate halides Sn 2 PO 4 X (X = F, Cl)

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  4. Cs2Bi2OSi2O7: A Promising Bismuth Silicate Nonlinear Optical Crystal with Face-Sharing BiO5 Polyhedra Exhibiting Strengthened Second Harmonic Generation Response and Birefringence

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  5. Exploration of the Crystal Structure and Thermal and Spectroscopic Properties of Monoclinic Praseodymium Sulfate Pr2(SO4)3

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

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