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RESEARCH PAPER · Journal of the American Chemical Society · 2024

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

Pengfei Li, Chun‐Li Hu, Yafeng Li, Jiang‐Gao Mao, Fang Kong

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Hg4(Te2O5)(SO4): A Giant Birefringent Sulfate Crystal Triggered by a Highly Selective CationOriginal(C 2 H 10 N 2 )[Zn 2 (HPO 4 ) 2 Cl 2 ]: substitution-activated new short-wave ultraviolet phosphate with pivotal dual-property enhancement5Designing promising ultraviolet (UV) birefringent crystals with different hydrogen-bonded phosphate frameworks18New ultraviolet transparent rare-earth borates with enhanced birefringence induced by cation chemical substitution15Noncentrosymmetric 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 modification45Strategically designed metal-free deep-ultraviolet birefringent crystals with superior optical properties18Hg16O12(NO3)6F2(H2O): A Mercury-Rich Nitrate Oxyfluoride with Diverse Triple-Coordinated Mercury-Based Units That Exhibits an Unparalleled [(Hg16O12F2(H2O))6+]∞ Cationic Framework and a Large Birefringence12The first Hg-based oxychalcogenide Sr2HgGe2OS6: Achieving balanced IR nonlinear optical properties through synergistic cation and anion substitution28Enhanced 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 Crystals8From Pb6(HPO3)(H2PO3)Cl9 to Pb6(HPO3)2Br8(H2O)·H2O: Halogen Regulation to Achieve Inorganic Metal Phosphite Halide Nonlinear Optical Material with Unprecedented Pb-Centered Polyhedral Units13Halogen Bond Unlocks Ultra‐High Birefringence73Halogen Bond Unlocks Ultra‐High Birefringence14Synthesis and characterization of novel double perovskite K2AgBiBr612Sulfate 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 Ordering4First copper (II) oxo-selenite-sulfate Cu4O(SeO3)(SO4)2 and the role of a lone electron pair in open framework crystal structure formation2Li2NaB3S2O12: A Deep-UV Transparent Borosulfate with Moderate Birefringence Derived from the [B3S2O12]∞ Infinite Chain Designed by the High Boron-to-Sulfur Ratio Strategy6Pb2TeV2O10: A Lead Vanadate Tellurate with Wide Mid-IR Transparency and Large Birefringence Induced by Multiple Birefringence-Active Groups11A Giant Optically Anisotropic Phosphate Driven by Mixed Valence Mercury Units22Stimulus-responsive multifunctions in a zinc( ii ) sulfate complex: photochromism, photoswitching nonlinear optical properties, amine detection and visual film application9From HgGa2(SeO3)4 to Hg2Ga(SeO3)2F: The first HgI-based selenite birefringent crystal triggered by linear groups and fluoride ions29[C3H7N6]3[B3O5(OH)2] and [C3H8N6]4[B12O19(OH)6]: Two Melamine Borates with Large Birefringence13BaPb2(CO3)2F2: Enhancing Birefringence by a Multiunit Synergy Effect9Balanced IR Nonlinear Optical Performance Achieved by Cation–Anion Module Cosubstitution in V-Based Salt-Inclusion Oxychalcogenides22Rational Design and Controlled Synthesis of High-Performance Inorganic Short-Wave UV Nonlinear Optical Materials150Breaking Performance Barriers in KBe 2 BO 3 F 2 (KBBF) Analogs by Functional Group Self‐Polymerization5Breaking Performance Barriers in KBe 2 BO 3 F 2 (KBBF) Analogs by Functional Group Self‐Polymerization48(C 6 H 5 N 2 )HgCl 3 : Discovery of a Polar Hg‐Based Hybrid Halide as Preeminent Nonlinear Optical and Birefringent Material Activated by π‐Conjugated Organic Cation Substitution38“All-four-in-one”: a novel mercury tellurite–nitrate Hg 3 (TeO 3 )(Te 3 O 7 )(NO 3 ) 2 exhibiting exceptional optical anisotropy29(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 range4BaSbBS 4 : a record-high-performance birefringent crystal identified by a target-driven closed-loop strategy28Bulk crystal growth and optical properties of a novel organic–inorganic hybrid nonlinear optical thiocyanate: [Mn(CH 3 CONH 2 ) 2 ] [Hg(SCN) 4 ]10Different p-block elements induce C 3 [111] octahedral distortion in titanium to generate an intense nonlinear effect14Hg 2 (HTe 2 O 5 )(PO 4 ): a novel phosphate crystal with enhanced birefringence enabled by the synergistic modification of multiple functional groups12Hg 2 (SeO 3 )(TeO 3 ): a novel tellurite–selenite birefringent crystal achieved by assembling multiple functional groups11Hg[CS(NH 2 ) 2 ] 4 (SiF 6 ): a fluorosilicate crystal with large birefringence achieved via multi-functional group modification6Highly stable and reversible birefringence switching triggered by thermally stimulated phase transition1K 2 Na(I 3 O 8 ) 3 : a promising mid-infrared birefringent material with two different structures of octaoxotriiodate( v ) polyanions1Significant enhancement in the birefringence of metal phosphite halides via the introduction of π-conjugated cations17β-LaTeBO 5 and RETeBO 5 (RE = Y, Gd, Tb): explorations of new optical materials in the RE( iii )–Te( iv )–B–O system7Design and Synthesis of Two Sn-Centered Mixed Halide Crystals with Enhanced Birefringence8Dual Lone Pair Strategy for High Birefringence in Antimony(III)-Based Tellurite Sulfates with Short-Wave UV Transparency10Designing Polar Covalent Hybrid Cadmium‐Based Chalcohalides Ultraviolet Nonlinear Optical Crystal with Strong Optical Anisotropy via Double‐Site Dual FBUs Tailoring25A 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 Strategy5From Holodirected to Hemidirected Coordination Activated by Oxygenation Strategy: A Facile Route to Long Wave Infrared Birefringent Crystal4From Holodirected to Hemidirected Coordination Activated by Oxygenation Strategy: A Facile Route to Long Wave Infrared Birefringent Crystal28Chalcophosphates: A plentiful source of infrared nonlinear optical materials42Engineering 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 Substitution6Tuning Birefringence in Supramolecular Mg-PDA Frameworks: Modulating Bonding and Layer Connectivity0Designed Metal‐Free Quasi‐1D Crystals with Giant Birefringence8Na[B3IO7(OH)] and Na2[B4IO9](IO3): Explorations of Boroiodates with Strong Second Harmonic Generation Response and Large Birefringence54Sb2(TeO4)(SO4): An Anhydrous Tellurite Sulfate with Large Birefringence and Enhanced Thermal Stability8Giant Birefringence Enabled by the Highly Anisotropic Linear IX 2 − (X = Cl, Br) Building Blocks6Giant Birefringence Enabled by the Highly Anisotropic Linear IX 2 − (X = Cl, Br) Building Blocks32Bridging 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 Crystals48La2Zn3(SeO3)6: A UV Selenite Crystal with Second-Harmonic Generation and Large Birefringence13Recent progress in structural design strategies of high-birefringence optical crystals54Ca 7 (TeO 3 ) 6 (MoO 4 ): A Promising Mid-Infrared Nonlinear Optical Crystal Activated via a Module-Oriented Dimensionality Reduction Strategy34(CH5N3S)2Pb5Br10 and (CH5N3S)Pb2Br4: Two Nonlinear Optical Lead Thiosemicarbazide Bromides with Diverse Pb-Centered Building Units10Giant Birefringence and Solar‐Blind Ultraviolet Transmission by Coordination‐Induced Assembly of π‐Conjugated Pyridine–Carboxylate8Giant Birefringence and Solar‐Blind Ultraviolet Transmission by Coordination‐Induced Assembly of π‐Conjugated Pyridine–Carboxylate24Planar [HgCl 3 ] and V‑Shaped [HgCl 2 ] Units Synergistically Creating a Prominent Halide Birefringent Crystal β ‐CsHg 2 Cl 5 with Wide‐Spectrum7[TeSeS 2 ] 2− : The First Heterotriple‐Chalcogenide Motifs Decode Giant Mid‐Far Infrared Birefringence18[TeSeS 2 ] 2− : The First Heterotriple‐Chalcogenide Motifs Decode Giant Mid‐Far Infrared Birefringence4Research progress and future prospect of chalcogenides with large optical anisotropy46Temperature dependence of polarizability, order parameters and dielectric properties of a nematic liquid crystals0Cs2CdV2O6Br2: A Mid-Infrared Nonlinear Optical Vanadate Containing Both d0/d10 Transition Metal Cations and Bromine Anions5Exceptional Second Harmonic Generation in Ultraviolet Nonlinear Optical Oxyfluoroniobate Crystals via Structural Fingerprint Optimization of Polar Chains22Exceptional Second Harmonic Generation in Ultraviolet Nonlinear Optical Oxyfluoroniobate Crystals via Structural Fingerprint Optimization of Polar Chains8Breaking the Birefringence Barrier in B–O Crystals via B–C π-scaffolding36A novel metal-free crystal demonstrating superior birefringence attributed to the synergistic interaction of dual π-conjugated units8Dual‐Sided Multidentate Coordination Strategy Enables Record Birefringence in UV‐Transparent Antimony‐Based Hybrid Crystals37Dual‐Sided Multidentate Coordination Strategy Enables Record Birefringence in UV‐Transparent Antimony‐Based Hybrid Crystals11Controlling d10 Metal in Phenylthiourea‐Based Hybrid Metal Halides to Actualize Dimensional Transformation and Significantly Improve the Birefringence11CsICl 2 : A Record-Birefringent Inorganic Crystal with Ultrawide Infrared Transparency Enabled by Linear Interhalogen ICl 2 – Units36A strategy to achieve giant optical anisotropy via integrating linear pseudohalogen and stereochemical active lone pair cation6Optimizing the Hydrogen-Bond Network Drives Cadmium Ce(IV) Fluoride Hydrate with Significantly Enhanced Optical Anisotropy8Achieving the birefringence-bandgap trade-off: Hydrogen-bond engineered biuret-cyanurate14Hydrogen Bond-Assisted Structural Regulation Enables Large Birefringence in Two Antimony Oxalofluoride Crystals5Low‐Dimensional Organic–Inorganic Hybrid Metal Halide with Large Optical Anisotropy9Achieving large birefringence in oxalate crystals by a hydrogen bond-directed strategy1(CN4H7)H2C3N3S3: Trithiocyanurate Exhibiting Giant Optical Anisotropy via Weak Interaction-Mediated Functional Module Alignment3Pioneering sulfophosphite crystals: Co-assembly of phosphite and sulfate units in novel inorganic architectures0Five-Membered [C 5 O 5 ] 2 – Rings as Birefringence-Active Genes for Ultrabirefringent Crystals27LnEuGa3OS6 (Ln = La, Pr, Nd): three dual rare earth metal-based oxychalcogenides with good IR nonlinear optical performances1Assembly of Highly Polarizable “Linkers” with Heteroleptic Groups for Inducing Large Optical Anisotropy in Ba2SnIIGe3O8S and Ba3SnIIGe3O2S82CsGaGe₃Se₈: Enhanced optical anisotropy and bandgap via cation-substitution-driven dimensionality reduction0K 2 GdB 3 O 6 F 2 : A Promising Short-Wave UV Birefringent Crystal via Optimized Assembly of π-Conjugated [B 3 O 6 ] Groups8Sulfonated Module Aggregation for Ultrahigh Birefringence in Aqueous-Processable Crystals26π-Conjugated unit bridge for giant second-harmonic generation and birefringence in hybrid materials with dual heteroleptic polyhedra5Stepwise Substitution Strategy for Beryllium-Based Selenites with Enhanced SHG Response, Moderate Birefringence, and Short UV Cutoff Edges6Hybrid Zinc‒Based Halides with Giant Optical Anisotropy via Protonation‒Engineered π ‒Conjugated Organic Group24Ba 3 S[SnOS 3 ] and [Ba 2 Sn]S[Ge 2 O 7 ]: two antiperovskite oxychalcogenides with good IR nonlinear optical performances2Ag(Te 2 O 3 )(PO 4 ): Linear and Nonlinear Optical Properties of a Noncentrosymmetric Phosphotellurite with P–O–Te Connection1ZnGa(SeO 3 ) 2 F: a UV transparent birefringent crystal explored in M( ii )–IIIA–selenite–F systems2Chiral-Unit-Driven Short-Wave Ultraviolet Nonlinear Optical Acetates with Balanced Overall Optical Properties3LiV 3 Se 2 O 12 : A Promising Giant‐Birefringent Crystal Enabled by Significant Structural Distortion3Cationic‐Dual‐Modulated Linear and V‐Shaped Birefringent‐Active Unit Generates Remarkable Birefringence6Synthesis, Crystal Growth, Linear, and Nonlinear Optical Properties of Water-Grown Giant Optical Anisotropic Thiocyanates ABi(SCN) 4 (A = Rb, Cs)3A mercury-based selenite with wide bandgap and moderate birefringence via cation substitution and partial fluorination1Achieving record birefringence in metal-free semiorganic sulfate crystals via tetrahedral anionic group substitution0Double second-order Jahn–Teller strategy driven NLO response in sulfate crystal Nb 2 O 2 (TeO 3 ) 2 (SO 4 ) with a large birefringence1From 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 modulation8LiHgTeO 3 : a Hg( i )-containing tellurite crystal with typical Hg–Hg bonds0中红外氧化物非线性光学晶体研究进展（特邀）0InO6X (X = Cl, Br): distinct functional motif family for nonlinear optical materials5[Hg3Se2]2- cluster drives giant optical anisotropy and broad infrared transparency16Halogen‐Bond Coupled Halogenated‐π‐Conjugation Enables Giant Birefringence in Hydrogen‐Bonded Organic Frameworks13Unit Symmetry‐Breaking and Layered Linear Ordering Enabling Superior Short‐Wave Ultraviolet Birefringent Crystal8Unit Symmetry‐Breaking and Layered Linear Ordering Enabling Superior Short‐Wave Ultraviolet Birefringent Crystal2Bonding-type-driven structural transformation toward novel fluoroiodosulfates: Achieving non-centrosymmetry and enhanced optical properties in K2(IO3F)SO30Unveiling the Superior Birefringence Property of a Record‐Birefringent Crystal with Unique Building Block12Unveiling the Superior Birefringence Property of a Record‐Birefringent Crystal with Unique Building Block4Unlocking Strong SHG Response and Large Birefringence in Hybrid Antimony Halides via a Three-in-One Strategy7An UV Transparent Metal‐Free Sulfate With Giant Birefringence Enabled by Optimal Structural Anisotropy4V-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 Crystals11[Ba2K][Br][SiS4]: An antiperovskite-type chalcohalide with simultaneously enhanced birefringence and band gap via cation-anion co-substitution0Rigid‐Flexible Coupling Units Enable Robust Large Birefringence2Recent Progress in Hg-Based Oxysalt Crystals for Nonlinear Optics and Birefringence Applications5From Coplanarity to Coaxiality: A Linearity-Oriented Design Paradigm for Ultrahigh Ultraviolet Birefringent Inorganic Crystals4Metal tellurite oxides: Lone-pair-enabled coordination chemistry, polymerized architectures, and functional materials opportunities1Steric hindrance and hydrogen-bond networks synergistically directing molecular alignment for high-performance ultraviolet birefringent1Record‐High Birefringence with Ultralow Dichroic Loss Realized by Cation‐Templated Engineering Ordered Assembly of Linear Birefringent‐Active Unit6Lock‐and‐Key Assembly Enables Record Birefringence in Monocyclic π‐Conjugated Crystals via Spatial Confinement of Linear Polyhalide5Lock‐and‐Key Assembly Enables Record Birefringence in Monocyclic π‐Conjugated Crystals via Spatial Confinement of Linear Polyhalide0K 2 ZrSi 2 O 7 with a Wide Transmission Range and Enhanced Birefringence Induced by the d 0 -TM Zr-Based Units2Bridging Motifs Induced Ordered Arrangement Contributing Large Birefringence for Hg 4 BiQ 2 Cl 5 (Q═S, Se)1Rb 2 ZnGe 3 Se 8 : A Large-Birefringence Layered Chalcogenide Enabled by Anisotropic Electrons in Tetrahedral Units0Unlocking Structural Anisotropy by Guest-Symmetry Modulation Strategy to Achieve Giant Birefringence in Molecular Crystals0Unlocking Nonlinear Optics and Photoluminescence with Simultaneous Enhancement of Bandgap and Birefringence in Hybrid Sb-Based Halides2Bioinspired Subnanowire‐Based Optical Devices With Programmable Polarization Irisations Through Photocuring 3D Printing0Exceptional Solar‐Blind Birefringence Engineered by Complementary Hydrogen‐Bond Ordering of π‐Conjugated Units0Heavy‐Halide Coordination and Lattice‐Confined Molecular Alignment Enable Giant Birefringence in Hybrid Metal Halides0AVP2S7 (A = K, Rb): Dual-Optimized Infrared Nonlinear Optical Thiophosphates via Heterovalent-Substitution-Driven Symmetry Breaking and Reinforced Interlayer Interactions0Designing Novel Solar‐Blind Ultraviolet Nonlinear Optical Crystals Based on Local Proton Distribution Complementary Effect0Designing Novel Solar‐Blind Ultraviolet Nonlinear Optical Crystals Based on Local Proton Distribution Complementary Effect0Non-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) units1EuMn6Ga6S16: A Wide Bandgap Europium-Based Nonlinear Optical Sulfide0Laporte Selection Rule Induced the Suppression of d ‐ d Transitions and Vacancies Enhanced the Second Harmonic Generation in I 4¯‐MnGa 2 S 40Cation-Modulated Activation of Linear Units in an Ordered Arrangement Achieves the Largest Optical Anisotropy in Wide-Bandgap Metal Chalcogenides0Mixed‐Valence Engineering in Ge 2+ Chalcogenides: Structural Modulation for Balanced Infrared Nonlinear Optics0

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

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

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  5. 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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