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RESEARCH PAPER · Angewandte Chemie International Edition · 2021

[Ag(NH3)2]2SO4: A Strategy for the Coordination of Cationic Moieties to Design Nonlinear Optical Materials**

Yi‐Chang Yang, Xin Liu, Jing Lu, Li‐Ming Wu, Ling Chen

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[Ag(NH3)2]2SO4: A Strategy for the Coordination of Cationic Moieties to Design Nonlinear Optical Materials**OriginalZn(NH 3 )CO 3 : a “three-in-one” UV nonlinear optical crystal built by a polar molecule bonding strategy18Synergistic Effect of π-Conjugated [C(NH 2 ) 3 ] Cation and Sb(III) Lone Pair Stereoactivity on Structural Transformation and Second Harmonic Generation58An excellent lead oxyiodide with a strong second-harmonic generation response and a large birefringence induced by the oriented arrangement of highly distorted [PbO 4 I 2 ] polyhedra13APb 2 (C 7 H 3 NO 4 ) 2 I (A = K, Rb, Cs): rare stable nonlinear optical crystals with second-harmonic generation response and highly distorted lead core coordination polyhedra2Crystal Structure and Theoretical Analysis of Cs2Ca3(SO4)47Review of Heteroleptic Tetrahedra as Birefringent or Nonlinear Optical Motifs17Advances in second-order nonlinear optical sulfates38CsY(SO4)2·4H2O: A Deep-Ultraviolet Birefringent Crystal Induced by an Edge-Sharing Connection26Self-Assembled Nonlinear Optical Crystals Based on an Asymmetric Fluorenone Derivative17Modulating Two Pairs of Chiral Dy III Enantiomers by Distinct β-Diketone Ligands to Show Giant Differences in Single-Ion Magnet Performance and Nonlinear Optical Response35Noncentrosymmetric (C3H7N6)6(H2PO4)4(HPO4)·4H2O and Centrosymmetric (C3H7N6)2SO4·2H2O: Exploration of Acentric Structure by Combining Planar and Tetrahedral Motifs via Hydrogen Bonds37Hydrogen Bond-Driven Order–Disorder Phase Transition in the Near-Room-Temperature Nonlinear Optical Switch [Ag(NH3)2]2SO424Dual-Ligand-Oriented Design of Noncentrosymmetric Complexes with Nonlinear-Optical Activity11Chalcohalides: A Rising Type of Second‐Order Nonlinear Optical Materials28New lead-iodide formates with a strong second-harmonic generation response and suitable birefringence obtained by the substitution strategy8AIB3IIC3IIIQ8VI: A New Family for the Design of Infrared Nonlinear Optical Materials by Coupling Octahedra and Tetrahedra Units152LiRE(SO 4 ) 2 (RE = Y, Gd, Eu): noncentrosymmetric chiral rare-earth sulfates with very large band gaps21M(NH2SO3)2·xH2O (M = Ca, Pb, x = 0, 1, 4): Effect of Hydrogen Bonding on Structural Transformations and Second Harmonic Generation of Metal Sulfamates26Anisotropic structure building unit involving diverse chemical bonds: a new opportunity for high-performance second-order NLO materials181Breaking the bottleneck of simultaneously wide band gap and large nonlinear optical coefficient by a “pore reconstruction” strategy in a salt-inclusion chalcogenide26Dramatically improved optical anisotropy by realizing stereochemically active lone pairs in a sulfate system, K 2 SO 4 ·HIO 323Evaluating refractive index and birefringence of nonlinear optical crystals: Classical methods and new developments45Linear optical afterglow and nonlinear optical harmonic generation from chiral tin( iv ) halides: the role of lattice distortions37Silver(I) trifluoroacetate complexes with n-allylic derivatives of quinoline and isoquinoline: synthesis and crystal structure0The search for a maximum of the D–π–A paradigm for second order nonlinear optical molecular materials9A Rare‐Earth Selenite with Unexpectedly Well‐Balanced Ultraviolet Nonlinear Optical Functionality, Sc(HSeO 3 ) 331K2(H2O)WO3F2: A new nonlinear optical material with remarkable second-harmonic generation response and enhanced laser damage threshold9Inorganic Solid‐State Nonlinear Optical Switch with a Linearly Tunable Tc Spanning a Wide Temperature Range22Inorganic Solid‐State Nonlinear Optical Switch with a Linearly Tunable Tc Spanning a Wide Temperature Range2Unveiling the Superior Optical Properties of Novel Melamine‐Based Nonlinear Optical Material with Strong Second‐Harmonic Generation and Giant Optical Anisotropy74Sb4O3(TeO3)2(HSO4)(OH): An Antimony Tellurite Sulfate Exhibiting Large Optical Anisotropy Activated by Lone Pair Stereoactivity30Hg3(SeO3)2(SO4): A UV Nonlinear Optical Mercury Selenite Sulfate Constructed by Neat [Hg6O8(SeO3)4]∞ Layers and SO4 Tetrahedra27Multifunctional properties of a polar spin chain compound [N(C3H7)4][Cu(C8H4NO4)]·H2O exhibiting both one-dimensional magnetism and nonlinear optical activity15Cs4Zn5P6S18I2: the Largest Birefringence in Chalcohalide Achieved by Highly Polarizable Nonlinear Optical Functional Motifs21Zn 2 HgP 2 S 8 : A Wide Bandgap Hg‐Based Infrared Nonlinear Optical Material with Large Second‐Harmonic Generation Response75Nonlinear optical inorganic sulfates: The improvement of the phase matching ability driven by the structural modulation41Rational Design of Noncentrosymmetric Organic–Inorganic Hybrids with a π-Conjugated Pyridium-Type Cation for High Nonlinear-Optical Performance19Excellent Nonlinear Optical M[M4Cl][Ga11S20] (M = A/Ba, A = K, Rb) Achieved by Unusual Cationic Substitution Strategy20Enlargement of Bandgap and Birefringence in Nonlinear Optical Alkali‐Metal Sulfate Crystals by the Substitution of Asymmetrical Non‐π‐Conjugated Cation8From Layered Borate to Porous-Layered Aluminoborate7Designing Sulfate Crystals with Strong Optical Anisotropy through π‐Conjugated Tailoring51Designing Sulfate Crystals with Strong Optical Anisotropy through π‐Conjugated Tailoring11Antibacterial adsorptive membrane decorated via silver nanolayer for ammonia removal11Cu3BiS3: Two‐Dimensional Coordination Induces Out‐of‐Plane Phonon Scattering Enabling Ultralow Thermal Conductivity6Cu3BiS3: Two‐Dimensional Coordination Induces Out‐of‐Plane Phonon Scattering Enabling Ultralow Thermal Conductivity21Na 10 Zn(NO 3 ) 4 (SO 3 S) 4 : a nonlinear optical crystal combining inorganic π-conjugated and non-π-conjugated heteroanion groups8K(NH4)Zn2(PO4)2: a Beryllium-Free Sr2Be2B2O7 Derivative with Enhanced Interlayer Connectivity7Ag 2 [TeO 2 (OH) 4 ]: a nonlinear optical tellurate with balanced comprehensive performance2Design of alkali lead oxybromides with a strong second-harmonic generation response and large birefringence1Pb 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 strategies10The Birefringence Modulation in Short‐Wave Ultraviolet Sulfates with Functional π‐Conjugated Cations and Polymerized Heteroleptic Tetrahedral Anions18(C8H6BrN2O)NO3: A Hybrid Nonlinear Optical Crystal With an Appropriate Birefringence12A2Pb3[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 Units6Intramolecular Hydrogen Bonds Enhance Structure Coplanarity, Resulting in Significant Birefringence in Bridged-Bipyridine Halides7From CaBaM2F12 to K2BaM2F12 (M = Zr, Hf): Heterovalent Cation-Substitution-Induced Symmetry Break and Nonlinear-Optical Activity11The centrosymmetric to non-centrosymmetric transformation induced by alkaline-earth cations producing infrared nonlinear optical AeMn6Ga6S16 (Ae = Ca, Sr)13Noncentrosymmetric Crystal [C10H8NO2]2SiF6·H2O with Large Birefringence12High second-order nonlinearity in single-domain tetragonal PMN-PT single crystal10NaK5La2(SO4)6: Enhanced Birefringence of Multiple-Alkali Metal Sulfate Systems via Rare Earth Metal-Centered Polyhedra5Sulfate 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 Ordering4Porous organic cages as a novel platform for second harmonic generation19Looking Back the Nonlinear Optical Crystals in a Functionalized Unit's Perspective109Cationic Coordination Modification Drives Birefringence and Nonlinear Effect Double Lifting in Sulfate4A strongly birefringent sulfate crystal with a wide second-harmonic generation phase-matching range4Structure modulation by cationic modification of sulfates using planar CS(NH 2 ) 25Cationic Modification in Hybrid Iodates: A Pathway to Superior Performance12Strong Second‐Harmonic Generation Responses in Salt‐Inclusion Oxychalcogenides Enabled by the Highly Distorted Polyhedra with Mixed‐Anions4Sb2(TeO4)(SO4): An Anhydrous Tellurite Sulfate with Large Birefringence and Enhanced Thermal Stability8Bridging 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 Crystals48From AgHgI(SO4) to AgHg3I3.2Cl1.8(SO4): Symmetry Breaking of the Belousovite‐Type Topology by Mixed Halides to Achieve Strong Nonlinear Optical Effect14Unravelling the impact of octahedral distortion and non-covalent interactions on the hyperpolarizabilities of Co(II) and Ni(II) coordination complexes with uridine nucleotide11Effect of NH3 on the Nature of Ag‐Nanoparticles Prepared via the Borohydride Reduction0Metal Chloride‐Iodate Nonlinear Optical Materials via Direct Chlorination of Centrosymmetric Metal Iodate Crystals0Ag(Te2O3)(PO4): The first Ag-containing phosphate-tellurite nonlinear optical crystal featuring novel zigzag layered structure0Remarkable Birefringence Enhancement Enabled by π-Conjugated Cyanoguanidine Group Based on Anisotropic Molecule Coordination Approach8pH‐Regulated Ring‐Opening/Closing Transformation in Polyoxometalates Enables High‐Performance Nonlinear Optical Crystals13Heterocationic strategy to design a nonlinear optical crystal with a polar anti-perovskite structure7Tailoring linear and nonlinear optical properties of 2D Sc 2 C MXenes via surface termination modulation0RbLa(SO 4 ) 2 : A KBBF-like Deep-UV Transparent Rare Earth Sulfate with Strong SHG Response and High Thermal Stability Enabled by Multicomponent Structural Design2Helical Mn(II)-based enantiomers based on lactic derivatives with ferroelectric and nonlinear optical properties3The Achievement of a Strong Second Harmonic Generation Response and a Large Birefringence in Sulfates4An Ultraviolet Transparent Nonlinear Optical Crystal Assembled from a Polarizable Tetrahedral Unit1

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  2. Synergistic Effect of π-Conjugated [C(NH 2 ) 3 ] Cation and Sb(III) Lone Pair Stereoactivity on Structural Transformation and Second Harmonic Generation

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  19. Anisotropic structure building unit involving diverse chemical bonds: a new opportunity for high-performance second-order NLO materials

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

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

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  50. 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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