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RESEARCH PAPER · Angewandte Chemie International Edition · 2023

Recent Development of Sn II , Sb III ‐based Birefringent Material: Crystal Chemistry and Investigation of Birefringence

Shujuan Han, Abudukadi Tudi, Wenbin Zhang, Xueling Hou, Zhihua Yang, Shilie Pan

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Recent Development of Sn II , Sb III ‐based Birefringent Material: Crystal Chemistry and Investigation of BirefringenceOriginal(C 5 H 6.16 N 2 Cl 0.84 )(IO 2 Cl 2 ): a birefringent crystal featuring unprecedented (IO 2 Cl 2 ) − anions and π-conjugated organic cations56Anisotropic structure building unit involving diverse chemical bonds: a new opportunity for high-performance second-order NLO materials181C 3 N 6 H 7 SO 3 NH 2 : non-π-conjugated tetrahedra decoupling π-conjugated groups achieving large optical anisotropy and wide band gap29From CdPb 8 (SeO 3 ) 4 Br 10 to Pb 3 (TeO 3 )Br 4 : the first tellurite bromide exhibiting an SHG response and mid-IR transparency21Heteroanion-introduction-driven birefringence enhancement in oxychalcogenide Ba 3 M II Ge 3 O 2 S 8 (M II = Mn, Cd)19Mg 2 Pb 2 Si 2 O 7 F 2 : a new lead-containing alkali earth metal silicate fluoride with a short cutoff edge2Stereochemically active lone-pair-driven giant enhancement of birefringence from three-dimensional CsZn 4 Ga 5 Se 12 to two-dimensional CsZnAsSe 319Synthesis, structure and characterization of Cd 2 TeO 3 Cl 2 with unprecedented [Cd 2 O 6 Cl 4 ] octahedral dimers5Ultraviolet Crystal with Strong Optical Nonlinearity by Creating Halogen-Centered Secondary Building Blocks15Cs4Zn5P6S18I2: the Largest Birefringence in Chalcohalide Achieved by Highly Polarizable Nonlinear Optical Functional Motifs21Three Borates Belonging to the A(I)7Ae(II)Re(III)2B15O30 Family as Promising Nonlinear Optical Crystals12A Two‐Dimensional Hybrid Perovskite With Heat Switching Birefringence47A Two‐Dimensional Hybrid Perovskite With Heat Switching Birefringence7YSO4F·H2O: A Deep-Ultraviolet Birefringent Rare-Earth Sulfate Fluoride with Enhanced Birefringence Induced by Fluorinated Y-Centered Polyhedra19Designing Sulfate Crystals with Strong Optical Anisotropy through π‐Conjugated Tailoring51Designing Sulfate Crystals with Strong Optical Anisotropy through π‐Conjugated Tailoring11Two van der Waals Layered Antimony(III) Phosphites as UV Optical Materials11Vanadate Crystals with an Enhanced Birefringence and a Broadened Transparency Spectrum through Controlled [VO3]∞ Chain Arrangements and Alkali Metal Cation Introduction4AGe2O4Q (A = Ba, Sr; Q = S, Se): A series of heteroanionic oxychalcogenides with large birefringence9PbTeB 4 O 9 : a lead tellurium borate with unprecedented fundamental building block [B 4 O 10 ] and large birefringence12CsSn2(HPO3)2I: The first inorganic metal phosphite iodide as a promising birefringent material exhibits a large birefringence with ideally layered framework24C(NH2)3Cd(C2O4)Cl(H2O)·H2O and BaCd(C2O4)1.5Cl(H2O)2: Two Oxalate Chlorides Obtained by Chemical Scissors Strategy Exhibiting Low-Dimensional Structural Networks and Balanced Overall Optical Properties14(C(NH2)3)2(I2O5F)(IO3)(H2O) and C(NH2)3IO2F2: Two Guanidine Fluorooxoiodates with Wide Band Gap and Large Birefringence20(C 13 N 3 H 14 ) 2 MBr 4 (M = Zn, Cd): two novel hybrid metal halides with balanced integrated nonlinear optical performance31[(C 5 H 6 N 2 ) 2 H](Sb 4 F 13 ): a polyfluoroantimonite with a strong second harmonic generation effect60[Sn 3 OF]PO 4 vs. [Sn 3 F 3 ]PO 4 : enhancing birefringence by breaking the R 3 symmetry and realigning lone pairs12A highly birefringent metal-free crystal assembled by cooperative non-covalent interactions30Achieving strong second harmonic generation effects induced via dimensional increase of PbX 6 octahedra and halogen substitutes in (C 10 H 11 N 3 )PbX 4 (X = Cl or Br)26Alkali-metal isocyanurate Cs 3 (H 2 C 3 N 3 O 3 ) 3 (H 3 C 3 N 3 O 3 )·3H 2 O: synthesis and characterization0Exploration of antimony( iii ) oxyhalides via single-site substitution in quest of large birefringence10Hydrogen bonding bolstered head-to-tail ligation of functional chromophores in a 0D SbF 3 ·glycine adduct for a short-wave ultraviolet nonlinear optical material32New antimony fluorooxoborates with strong birefringence and unprecedented structural characterisation19Novel antimony phosphates with enlarged birefringence induced by lone pair cations4Partial substitution with a significant effect: coexistence of a wide band gap and large birefringence in the oxychalcogenide AEGe 2 O 4 Se (AE = Sr and Ba)17Pb 2 (SeO 3 )(SiF 6 ): the first selenite fluorosilicate with a wide bandgap and large birefringence achieved through perfluorinated group modification45Research progress in optical materials with cationic organic planar π-conjugated groups containing CN bonds34Exceptional Optical Anisotropy Enhancement Achieved Through Dual‐Ions Cosubstitution Strategy in Novel Hybrid Bismuth Halides23Two Short-Wave UV Antimony(III) Sulfates Exhibiting Large Birefringence18Stereochemically Active Lone Pair Leads to Birefringence in the Vacancy Ordered Cs3Sb2Cl9 Perovskite Single Crystals13Enhancement of Birefringence in π-Conjugated Oxyfluorides Achieved via van der Waals Layered Structural Optimization10The Spin–Orbit Effect on the Electronic Structures, Refractive Indices, and Birefringence of X2PO4I (X = Pb, Sn, Ba and Sr): A First-Principles Investigation6Layered (C5H6ON)2[Sb2O(C2O4)3] with a large birefringence derived from the uniform arrangement of π-conjugated units11(C 8 H 7 N 2 O 2 ) 2 [Bi 2 Br 8 ]·2H 2 O and (C 8 H 7 N 2 O 2 ) 6 [Bi 2 Cl 10 ]Cl 2 ·2H 2 O: Exploring Birefringent Crystals in Hybrid Halide Systems5PbBeB2O5: A High-Performance Ultraviolet Nonlinear-Optical Crystal with Functional [BeB2O8]8– Group3Old tree blossoms anew: Research progress on the structures and optical properties of ultraviolet selenites56Sulfate 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 Ordering4Photoinduced Bending and Curling Motions in Molecular Microcrystals of Naphthyl Meldrum’s Acid Derivative Based on E-to-Z Photoisomerization7Cu(I)‐Induced ‘Click Reaction’ Involving Coordination and Covalent Assembly of Hybrid Borates for the Electrocatalytic CO 2 Reduction4Cu(I)‐Induced ‘Click Reaction’ Involving Coordination and Covalent Assembly of Hybrid Borates for the Electrocatalytic CO 2 Reduction11Pb2TeV2O10: A Lead Vanadate Tellurate with Wide Mid-IR Transparency and Large Birefringence Induced by Multiple Birefringence-Active Groups11(C10N2H10)(HI2O6)(HIO3)(IO3): A Birefringent Material Featuring Large π-Conjugated Organic Cation and Two Types of Iodate Anions2A Giant Optically Anisotropic Phosphate Driven by Mixed Valence Mercury Units22From [Ba3S][GeS4] to [Ba3CO3][MS4] (M = Ge, Sn): Enhancing optical anisotropy in IR birefringent crystals via functional group implantation11Synthesis, structure and characterizations of the first alkali-metal/alkaline-earth-metal oxalatophosphate Na4Mg3(HPO4)4(C2O4)·2H2O3A new alkali-earth metal oxalatohydrophosphate crystal Ba2(C2O4)(HPO4): Synthesis, structure, optical and thermal properties5BaPb2(CO3)2F2: Enhancing Birefringence by a Multiunit Synergy Effect9Birefringence Disparity Induced by Synergistic Effects of Stereochemically Active Lone Pairs19(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(C 5 N 2 H 7 )IO 2 F 2 and (C 3 N 6 H 8 )(IO 2 F 2 ) 2 : two new organic–inorganic hybrid fluoroiodate birefringent crystals7(CN 4 H 7 ) 2 SO 4 ·H 2 O: high-performance metal-free ultraviolet birefringent crystal with KBBF-like configuration5Cation tuning in anionic framework hydroborates: tailored deep-ultraviolet optical crystals with large birefringence1Deep-ultraviolet nonlinear-optical crystals LiBePO 4 and BeP 2 O 6 synthesized by ionic potential modulation towards uniform arrangement of PO 4 groups5Four noncentrosymmetric molybdophosphates discovered by a chemical substitution strategy4Greatly enhancing birefringence of fluorosilicates through the synergetic effect of functional units13Hg 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 groups11M 3 MoO 4 (HCO 3 ) (M = Rb and Cs): cation-tuned synthesis of two noncentrosymmetric molybdate-carbonates with isolated [MoO 4 ] and [HCO 3 ] groups0RbB 7 O 10 (OH) 2 and NaB 11 O 16 (OH) 2 : alkali metal hydroxyborates with two-dimensional layered structures and large birefringence1Structural chemistry of antimony( iii ) oxalates with lone pairs: polyhedral distortion [SbO 4 F 2 ], π-conjugation [C 2 O 4 ], and birefringence tuning1β-LaTeBO 5 and RETeBO 5 (RE = Y, Gd, Tb): explorations of new optical materials in the RE( iii )–Te( iv )–B–O system7BaFS: Birefringence Enhanced by the Transformation from Optical Isotropy to Anisotropy via Interlayer Anion Substitution8Design and Synthesis of Two Sn-Centered Mixed Halide Crystals with Enhanced Birefringence8SnHPO4: A Layered Tin(II) Phosphate with Enhanced Birefringence51Dual Lone Pair Strategy for High Birefringence in Antimony(III)-Based Tellurite Sulfates with Short-Wave UV Transparency10Pb 4 O 3 I 2 : A Lead Oxyhalide IR Optical Crystal with an Unprecedented 1 ∞ [O 3 Pb 4 ] Chain Featuring a Wide Transmittance Range and Large Birefringence3From 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 Crystal28Enhanced Birefringence and Excellent Thermal Stability in Two Tellurium(IV) Vanadates: KTeOVO4 and Ca2TeV2O95Na2MP3O9 (M = K, Rb): Two Potential Zero-Order Waveplate Materials with DUV Cutoff Edges2Designed Metal‐Free Quasi‐1D Crystals with Giant Birefringence8Metal Cation Engineered UV Birefringent Crystals in π‐Conjugated Sulfonates with Record‐High Optical Anisotropy17Sb2(TeO4)(SO4): An Anhydrous Tellurite Sulfate with Large Birefringence and Enhanced Thermal Stability8Hg3(TeO3)2(NO3)2 and Hg3(Te2O5)2(NO3)2: The First Two Hg‐Based Tellurite Nitrate Unit‐Mixed Crystals with Large Optical Anisotropy16Giant 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 Blocks32All-three-in-one: Pb2(H2PO4)2(C2O4) significantly enhanced birefringence in phosphate materials4Recent Research Progress of Antimony‐Based Two‐Dimensional Materials for Electronics and Optoelectronics20Synthesis, structure and properties of a new nitrate halide optical material: Cs3Zn(NO3)Br40Reversal Enhancement of Birefringence by Stereochemically Active Lone Pairs in Sn(II)-Based Mixed Halides0CsICl 2 : A Record-Birefringent Inorganic Crystal with Ultrawide Infrared Transparency Enabled by Linear Interhalogen ICl 2 – Units36A3ZnNO3X4 (A = Rb, NH4, X = Cl, I): Regulating Cations and Halides Yields Birefringent Crystals with Significantly Enhanced Optical Anisotropy5(CN4H7)H2C3N3S3: Trithiocyanurate Exhibiting Giant Optical Anisotropy via Weak Interaction-Mediated Functional Module Alignment3Anion-Ordered [B3O5(OH)2] Induced by Crystal Water with Deep Ultraviolet Transparency and Large Birefringence in Boron-Rich Borophosphates4Regulating the coplanarity of π-conjugated units through hydrogen bonding in FAHC2O4 and FAH2C3N3S3 crystals5[HgX 2 ] Linear Group Enabled Ultraviolet Birefringent Crystal RbHg 5 Br 11 with Strong Optical Anisotropy and Wide Bandgap12Assembly of Highly Polarizable “Linkers” with Heteroleptic Groups for Inducing Large Optical Anisotropy in Ba2SnIIGe3O8S and Ba3SnIIGe3O2S82Triple Integration of π‐Conjugated Building Blocks: Unprecedented Assembly for Large Optical Anisotropy11LiPb 3 GeS 4 Cl 3 : Quasi‐T 2 ‐Supertetrahedral 3D Framework Enabling Superior Optical Performance14Remarkable 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 Crystals1pH‐Regulated Ring‐Opening/Closing Transformation in Polyoxometalates Enables High‐Performance Nonlinear Optical Crystals13K 6 Mo 8 PO 29 OH·H 2 O and K 6 Mo 5 P 2 O 23 ·7H 2 O: strongly distorted [MoO 6 ] octahedral groups effectively enhance birefringence0[C(NH 2 ) 3 ] 2 PO 3 (OH): A Deep-Ultraviolet Birefringent Crystal Enabled by Synergy of π-Conjugated Cations and Heteroleptic Tetrahedra2LiV 3 Se 2 O 12 : A Promising Giant‐Birefringent Crystal Enabled by Significant Structural Distortion3[Al(H 2 O) 6 ](NO 3 )Cl 2 : achieving parallel arrangement of functional units and birefringence enhancement through free halogen-mediated structural regulation0[ICl 4 ] − : A large anisotropic planar anion group produces giant birefringence2KTeOPO 4 and NH 4 SnClSO 4 : two new KTiOPO 4 derivatives as birefringent crystals featuring enhanced optical anisotropy0Layered perovskite-like nitrates A 2 Ca(NO 3 ) 2 Cl 2 (A = Rb, Cs) as ultraviolet birefringent optical materials3Polarization optical metrology for linear birefringence in transparent anisotropic medium0Syntheses, structures and optical properties of two new cadmium antimonites: Cs 4 Cd(SbF 5 ) 3 (H 2 O) 2 and Cd[Sb 7 O 10 (OH)](SO 4 )0The condensation of π-conjugated units: a new paradigm for designing high-performance optical crystals4Halogen‐Bond Coupled Halogenated‐π‐Conjugation Enables Giant Birefringence in Hydrogen‐Bonded Organic Frameworks13Anion-Centered Engineering for Simultaneously Enhancing Birefringence and Band Gap in Chalcogenides1[C(NH 2 ) 3 ]SbCl 4 : An NLO Material with Enhanced Second Harmonic Response and Birefringence3From [C(NH2)3]2[Sn2(C2O4)3]·2H2O to [C(NH2)3]4[Sn(C2O4)2]2·H2O: Uneven-substitution-activated polar stannous oxalate with balanced bandgap and birefringence0Record‐Short Phase Matchability of Silicate: Charge‐Driven Lattice Distortion Enables Deep‐UV Phase Matching and Strong Optical Nonlinearity0V-Shaped Pseudo-Chains Coupled with Lone-Pair-Distorted [GeX 3 ] − Units Enable Large Birefringence in Ge(II) Hybrid Halides2NaNO 3 [(NH 2 ) 2 SO 2 ] 2 : A Halogen‐Free KBBF‐Type Nitrate Crystal with Record Birefringence for Ultraviolet Applications0Steric hindrance and hydrogen-bond networks synergistically directing molecular alignment for high-performance ultraviolet birefringent1Engineering Multiple Hydrogen‐Bond Sites With D‐π‐A Motifs for Strong Optical Nonlinearity and Giant Birefringence in Organic‐Inorganic Halides4Redox‐Driven Strategy Enabling Leapfrog Enhancement of Birefringence in Layered Tin‐Based Optical Crystals1The novel Zn-based ultraviolet birefringent crystals combined both large birefringence and wide bandgap2Local Aromatic Overlap Microregulation Enables Birefringence Enhancement in Isocompositional Hybrid Antimony Halides1Cation-Modulated Activation of Linear Units in an Ordered Arrangement Achieves the Largest Optical Anisotropy in Wide-Bandgap Metal Chalcogenides0Domino‐Effect Amplification via Covalent‐Chain Engineering for Giant Birefringence in NaAsQ 2 (Q = S, Se) Crystals0MAlB3O6F2 (M = Ca and Pb): Two New Fluoroaluminoborates Featuring π-Conjugated [BO3] and [AlO4F2] Units with Large Birefringence0[La3Br][GeS4]2: Cationic-Moiety-Guided Strategy Enables Record Birefringence and Broad Optical Window0

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  1. (C 5 H 6.16 N 2 Cl 0.84 )(IO 2 Cl 2 ): a birefringent crystal featuring unprecedented (IO 2 Cl 2 ) − anions and π-conjugated organic cations

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

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  3. C 3 N 6 H 7 SO 3 NH 2 : non-π-conjugated tetrahedra decoupling π-conjugated groups achieving large optical anisotropy and wide band gap

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  4. From CdPb 8 (SeO 3 ) 4 Br 10 to Pb 3 (TeO 3 )Br 4 : the first tellurite bromide exhibiting an SHG response and mid-IR transparency

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  5. Heteroanion-introduction-driven birefringence enhancement in oxychalcogenide Ba 3 M II Ge 3 O 2 S 8 (M II = Mn, Cd)

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  6. Mg 2 Pb 2 Si 2 O 7 F 2 : a new lead-containing alkali earth metal silicate fluoride with a short cutoff edge

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  7. Stereochemically active lone-pair-driven giant enhancement of birefringence from three-dimensional CsZn 4 Ga 5 Se 12 to two-dimensional CsZnAsSe 3

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  8. Synthesis, structure and characterization of Cd 2 TeO 3 Cl 2 with unprecedented [Cd 2 O 6 Cl 4 ] octahedral dimers

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  9. Ultraviolet Crystal with Strong Optical Nonlinearity by Creating Halogen-Centered Secondary Building Blocks

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  10. Cs4Zn5P6S18I2: the Largest Birefringence in Chalcohalide Achieved by Highly Polarizable Nonlinear Optical Functional Motifs

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  14. YSO4F·H2O: A Deep-Ultraviolet Birefringent Rare-Earth Sulfate Fluoride with Enhanced Birefringence Induced by Fluorinated Y-Centered Polyhedra

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  15. Designing Sulfate Crystals with Strong Optical Anisotropy through π‐Conjugated Tailoring

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  16. Designing Sulfate Crystals with Strong Optical Anisotropy through π‐Conjugated Tailoring

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  17. Two van der Waals Layered Antimony(III) Phosphites as UV Optical Materials

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  18. Vanadate Crystals with an Enhanced Birefringence and a Broadened Transparency Spectrum through Controlled [VO3]∞ Chain Arrangements and Alkali Metal Cation Introduction

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  19. AGe2O4Q (A = Ba, Sr; Q = S, Se): A series of heteroanionic oxychalcogenides with large birefringence

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  20. PbTeB 4 O 9 : a lead tellurium borate with unprecedented fundamental building block [B 4 O 10 ] and large birefringence

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  21. CsSn2(HPO3)2I: The first inorganic metal phosphite iodide as a promising birefringent material exhibits a large birefringence with ideally layered framework

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  22. C(NH2)3Cd(C2O4)Cl(H2O)·H2O and BaCd(C2O4)1.5Cl(H2O)2: Two Oxalate Chlorides Obtained by Chemical Scissors Strategy Exhibiting Low-Dimensional Structural Networks and Balanced Overall Optical Properties

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  23. (C(NH2)3)2(I2O5F)(IO3)(H2O) and C(NH2)3IO2F2: Two Guanidine Fluorooxoiodates with Wide Band Gap and Large Birefringence

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  25. [(C 5 H 6 N 2 ) 2 H](Sb 4 F 13 ): a polyfluoroantimonite with a strong second harmonic generation effect

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  27. A highly birefringent metal-free crystal assembled by cooperative non-covalent interactions

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  28. Achieving strong second harmonic generation effects induced via dimensional increase of PbX 6 octahedra and halogen substitutes in (C 10 H 11 N 3 )PbX 4 (X = Cl or Br)

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  29. Alkali-metal isocyanurate Cs 3 (H 2 C 3 N 3 O 3 ) 3 (H 3 C 3 N 3 O 3 )·3H 2 O: synthesis and characterization

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  30. Exploration of antimony( iii ) oxyhalides via single-site substitution in quest of large birefringence

    Inorganic Chemistry Frontiers · 2024-01-01

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  31. Hydrogen bonding bolstered head-to-tail ligation of functional chromophores in a 0D SbF 3 ·glycine adduct for a short-wave ultraviolet nonlinear optical material

    Chemical Science · 2024-01-01

    Zhiyong Bai, Jihyun Lee, Chun‐Li Hu, Guohong Zou, Kang Min Ok

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  32. New antimony fluorooxoborates with strong birefringence and unprecedented structural characterisation

    Chemical Communications · 2024-01-01

    Chenhui Hu, Mengfan Wu, Jian Wei Han, Zhihua Yang, Shujuan Han, Shilie Pan

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  33. Novel antimony phosphates with enlarged birefringence induced by lone pair cations

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  34. Partial substitution with a significant effect: coexistence of a wide band gap and large birefringence in the oxychalcogenide AEGe 2 O 4 Se (AE = Sr and Ba)

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    Mao‐Yin Ran, Shenghua Zhou, Wenbo Wei, A-Yang Wang, Xin‐Tao Wu, Hua Lin, Qi‐Long Zhu

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  35. 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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