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RESEARCH PAPER · Angewandte Chemie International Edition · 2020

α‐SnF 2 : A UV Birefringent Material with Large Birefringence and Easy Crystal Growth

Jingyu Guo, Abudukadi Tudi, Shujuan Han, Zhihua Yang, Shilie Pan

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α‐SnF 2 : A UV Birefringent Material with Large Birefringence and Easy Crystal GrowthOriginalSynergism of multiple functional chromophores significantly enhancing the birefringence in layered non-centrosymmetric chalcohalides20The synthesis, characterization, and theoretical analysis of (NH 4 ) 3 PbCl 52A new rare-earth borate birefringent crystal with quasi-two-dimensional [BO 3 ] layers23An organic–inorganic hybrid birefringent material with diverse functional groups38Barium fluoroiodate crystals with a large band gap and birefringence22BaTi(BO 3 ) 2 : an excellent birefringent material with highly coplanar isolated [BO 3 ] groups16Distinctive modulation of optical anisotropy by halogens in α/β-Cd–P–X (X = Cl, Br, and I)2RbMo 2 P 3 O 14 with large birefringence mainly induced by highly distorted [MoO 6 ] in uncommon [Mo 2 P 3 O 14 ] ∞ layers9AZn4(OH)4(C3N3O3)2 (A = Mg, Zn): Two Zn-Based Cyanurate Crystals with Various Cation Coordination and Large Birefringence22Li 4 MgGe 2 S 7 : The First Alkali and Alkaline‐Earth Diamond‐Like Infrared Nonlinear Optical Material with Exceptional Large Band Gap213Li4MgGe2S7: The First Alkali and Alkaline‐Earth Diamond‐Like Infrared Nonlinear Optical Material with Exceptional Large Band Gap15Sn2PO4I: An Excellent Birefringent Material with Giant Optical Anisotropy in Non π‐Conjugated Phosphate212Sn2PO4I: An Excellent Birefringent Material with Giant Optical Anisotropy in Non π‐Conjugated Phosphate22High thermopower and birefringence in layered mercury-based halides2Tin(II)-Induced Large Birefringence Enhancement in Metal Phosphates221D Chiral Lead Halide Perovskites with Superior Second‐Order Optical Nonlinearity100Helical {[HgS]} n Chain-Induced Balanced Nonlinear-Optical Performance for Trigonal Mercury Sulfide29Enhancement of band gap and birefringence induced via π -conjugated chromophore with “tail effect”28A 6 Mo 2 P 4 O 19 (A = Rb, Cs) and Rb 2 MoP 2 O 9 : new molybdophosphates with distinct polyanionic configurations5[C 3 N 6 H 7 ] 2 [B 3 O 3 F 4 (OH)]: a new hybrid birefringent crystal with strong optical anisotropy induced by mixed functional units85[C(NH 2 ) 3 ] 2 S 2 O 8 : combining delocalized and localized π-conjugate units to achieve strong optical anisotropy21Ba 2 Zn 2 B 6 O 13 : coplanar [B 2 O 5 ] in unnoted U-shaped [B 6 O 13 ] groups achieving large birefringence6Halogen regulation triggers structural transformation from centrosymmetric to noncentrosymmetric switches in tin phosphate halides Sn 2 PO 4 X (X = F, Cl)47Hg 2 (SeO 3 )(SO 4 ): the first sulfate selenite with large birefringence explored from d 10 transition metal compounds36KSb(BeF 3 )F 3 : a totally fluorine strategy for achieving wide bandgap and large birefringence23Large optical anisotropy differentiation induced by the anion-directed regulation of structures29LiSrSbS 3 : parallel configurations of lone pair electrons inducing a large birefringence16Na 4 Ga 8 S 14 : a Ga-enriched wide band gap ternary alkali-metal sulfide with unique [Ga 12 S 42 ] 12-membered rings2NH 4 (B 6 PO 10 (OH) 4 )·H 2 O: exhibiting the largest birefringence in borophosphates43Sn 9O 4Br 9X (X = Cl, Br): Two New Sn(II) Oxyhalides Exhibiting Large Birefringence Derived from Highly Distortive Polyhedra of Lone Pair Cations0High‐Performance Sulfate Optical Materials Exhibiting Giant Second Harmonic Generation and Large Birefringence21High‐Performance Sulfate Optical Materials Exhibiting Giant Second Harmonic Generation and Large Birefringence199From Pb(H 2 C 3 N 3 O 3 )(OH) to Pb(H 2 C 3 N 3 O 3 )F: Homovalent Anion Substitution-Induced Band Gap Enlargement and Birefringence Enhancement26HgTeO2F(OH): A Nonlinear Optical Oxyfluoride Constructed of Active [TeO2F(OH)]2– Pyramids and V-Shaped [HgO2]2– Groups36First-principles study of the influence of lone pair electrons and molecular groups on the birefringence of phosphate and fluorophosphate13Potential optical functional crystals with large birefringence: Recent advances and future prospects322Explorations of New SHG Materials in Mercury Iodate Sulfate System**9Two Indium Iodate–Nitrates with Large Birefringence Induced by Hybrid Anionic Functional Groups and Their Favorable Arrangements22Layered Perovskite-like Nitrate Cs2Pb(NO3)2Br2 as a Multifunctional Optical Material40Promising Deep‐Ultraviolet Birefringent Materials via Rational Design and Assembly of Planar π‐Conjugated [B(OH)3] and [B3O3(OH)3] Functional Species6Promising Deep‐Ultraviolet Birefringent Materials via Rational Design and Assembly of Planar π‐Conjugated [B(OH)3] and [B3O3(OH)3] Functional Species83Realization of Enlarged Birefringence from BaCdBe2(BO3)2F2 to NaMgBe2(BO3)2F via the Cation Size Effect as a Potential Deep-Ultraviolet Birefringent Material18NaBaBS3: A Promising Infrared Functional Material with Large Birefringence Induced by π-Conjugated [BS3] Units32Pressure induced modulations in the optoelectronic properties of Hg2Cl2 compound: Insights from the first-principle calculations11A new birefringent material, HfF2(IO3)2, with a large birefringence and improved overall performances achieved by the integration of functional groups19ZrF2(IO3)2 and RbGaF3(IO3): Two Promising Birefringent Crystals Featuring 1D Metal-Fluoride Cationic Chains and Wide Bandgaps22Sn3B10O17Cl2 Achieving Birefringence Enhancement by Stereochemical Activity Lone Pair9Li2PbB2O5: A Pyroborate with Large Birefringence Induced by the Synergistic Effect of Stereochemical Active Lone Pair Cations and π-Conjugated [B2O5] Groups14LiKCuP2O7: Cation substitution application with mixed-alkaline copper-containing pyrophosphate and magnetic properties2Rb 3 B 5 O 8 F 2 and K 0.6 Rb 2.4 B 5 O 8 F 2 : two new deep-ultraviolet transparent nonlinear optical fluorooxoborates designed by cation regulation13Noncentrosymmetric versus Centrosymmetric: Halogen Induced Variable Coordination Modes of Sn2+ and Structural Transition in Sn3B3O7X (X = Cl and Br)17(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 cations56C 10 H 6 NO 2 Cd(NO 3 )·2H 2 O: a birefringent crystal with an enlarged band-gap derived from covalent edge-sharing connection4Deep ultraviolet hydrogel based on 2D cobalt-doped titanate53Enhancement of birefringence and refractive index dispersion optimization from iodates to fluorooxoiodates1KRb 2 (NO 3 ) 2 Cl: a new birefringent crystal exhibiting a perovskite-related framework and a short cutoff edge6LiCs 3 AlB 7 O 14 : achieving enhanced optical anisotropy via [AlO 4 ] tetrahedron introduction to rearrange the anionic framework5Linear π-conjugated units of the D ∞h point group as superior ultraviolet birefringent units1Mg 2 Pb 2 Si 2 O 7 F 2 : a new lead-containing alkali earth metal silicate fluoride with a short cutoff edge2Synthesis and characterization of a new isoxazolone-based nonlinear optical crystal: MPMOI7The transformation of a zero-dimensional cluster into a one-dimensional chain structure achieving a dramatically enhanced birefringence in tin( ii )-based oxalates33Pb2Cl2(HPO3)(H2O) and Pb3Br2(HPO3)2: Two Phosphite Halides with 3D Structural Networks and Enlarged Birefringence18Organic Nonlinear Optical Crystals for Highly Efficient Terahertz-Wave Generation36Two Carboxylate-Cyanurates with Strong Optical Anisotropy and Large Band Gaps6Li3B8O13X (X = Cl and Br): Two New Noncentrosymmetric Crystals with Large Birefringence Induced by BO3 Units18Recent Development of Sn II , Sb III ‐based Birefringent Material: Crystal Chemistry and Investigation of Birefringence130Recent Development of SnII, SbIII‐based Birefringent Material: Crystal Chemistry and Investigation of Birefringence6Sn9O4Br9X (X = Cl, Br): Two new Sn(II) oxyhalides exhibiting large birefringence derived from highly distortive polyhedra of lone pair cations9Chain‐like [S x ] ( x =2–6) Units Realizing Giant Birefringence with Transparency in the Near‐Infrared for Optoelectronic Materials53Chain‐like [S x ] ( x =2–6) Units Realizing Giant Birefringence with Transparency in the Near‐Infrared for Optoelectronic Materials5A Hydrogen Bonded Supramolecular Framework Birefringent Crystal89A Hydrogen Bonded Supramolecular Framework Birefringent Crystal13Birefringence Regulation by Clarifying the Relationship Between Stereochemically Active Lone Pairs and Optical Anisotropy in Tin‐based Ternary Halides56Birefringence Regulation by Clarifying the Relationship Between Stereochemically Active Lone Pairs and Optical Anisotropy in Tin‐based Ternary Halides2ASb(SO4)2 (A = Rb, Cs): Two short-wave UV antimony sulfates exhibiting large birefringence43Mixed Alkali Metal and Alkaline Earth Metal Scandium Borate Birefringence Material with Layered Structure and Short Ultraviolet Cutoff Edge17Improved Birefringence Activated by Tetrahedra Decorated with a Single Linear Unit38Improved Birefringence Activated by Tetrahedra Decorated with a Single Linear Unit1Ultraviolet Crystal with Strong Optical Nonlinearity by Creating Halogen-Centered Secondary Building Blocks15(NH 4 ) 2 (I 5 O 12 )(IO 3 ) and K 1.03 (NH 4 ) 0.97 (I 5 O 12 )(IO 3 ): Mixed‐Valent Polyiodates with Unprecedented I 5 O 12 − Unit Exhibiting Strong Second‐Harmonic Generation Responses and Giant Birefringence22Ce(IO3)3F and Ce(IO3)2(NO3): Two Mixed-Anion Cerium Iodates with Good Nonlinear Optical and Birefringent Properties14K2Sr4(PO3)10: A Polyphosphate with Deep-UV Cutoff Edge and Enlarged Birefringence6Designing a Hybrid Perovskite with Enlarged Birefringence and Bandgap for Modulation of Light Polarization32Highly Birefringent d 0 Transition Metal Fluoroantimonite in the Mid Infrared Band: Order–Disorder Regulation by Cationic Size83Designing Sulfate Crystals with Strong Optical Anisotropy through π‐Conjugated Tailoring51Designing Sulfate Crystals with Strong Optical Anisotropy through π‐Conjugated Tailoring11Hydroxyl-Driven Enhanced Birefringence in Borophosphates3PbTeB 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 framework24Rational Design of the Alkali Metal Sn‐Based Mixed Halides with Large Birefringence and Wide Transparent Range44[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 interactions30Crystal clear: unveiling giant birefringence in organic–inorganic cocrystals33Designing excellent UV birefringent materials through the synergistic interaction of two highly distorted functional groups23Explorations of highly birefringent materials in the vanadium oxyfluoride–iodate system by fluoride ion modulation8HgBr 2 : an easily growing wide-spectrum birefringent crystal38K 2 MgMoP 2 O 10 and K 3 Mg 2 MoP 3 O 14 : two new molybdophosphates exhibiting different optical anisotropies induced by variable dimensionality of the anion framework4Na 4 Sn 4 (C 2 O 4 ) 3 F 6 and NaSnC 2 O 4 F·H 2 O: two tin( ii ) fluoride oxalates display large birefringence11NaVSeO 5 : synergistic combinations to synthesize excellent birefringent materials8Novel antimony phosphates with enlarged birefringence induced by lone pair cations4Pb 3.5 GeS 4 Br 3 : the first phase-matching thiogermanate halide infrared nonlinear optical material12RbSb(SO 4 )(H 2 PO 2 )F: a short-wave UV antimony( iii ) oxysalt with mixed-anions demonstrating enhanced birefringence11Simple aliovalent cation substitution to induce strong optical anisotropy enhancement in a rare thioantimonate( v ) family3Design of Deep-Ultraviolet Zero-Order Waveplate Materials by Rational Assembly of [AlO2F4] and [SO4] Groups9Sb4O5I2: Enhancing Birefringence through Optimization of Sb/I Ratio for Alignment of Stereochemically Active Lone Pairs18Screening Large Birefringent Materials via Halogen Regulation in Ternary d0-Transition Metal Oxyhalides8Exceptional Optical Anisotropy Enhancement Achieved Through Dual‐Ions Cosubstitution Strategy in Novel Hybrid Bismuth Halides23AX·(H2SeO3)n (A = K, Cs; X = Cl, Br; n = 1, 2): A Series of Ionic Cocrystals as Promising UV Birefringent Materials with Large Birefringence and Wide Band Gap20Synthesis, structures and properties of two new nitrate optical materials: Rb3ZnNO3Cl4 and Rb5Na(NO3)4Cl24Unearthing 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 Engineering4Giant Optical Anisotropy in a Covalent Molybdenum Tellurite via Oxyanion Polymerization43Design of deep-ultraviolet zero-order waveplate materials using LiB3O5 as the template8The Birefringence Modulation in Short‐Wave Ultraviolet Sulfates with Functional π‐Conjugated Cations and Polymerized Heteroleptic Tetrahedral Anions18C(NH2)3MoO3(IO3): A Molybdenyl Iodate with Giant Birefringence Designed via a Cation–Anion Synergetic Interaction Strategy36[C(NH2)3]6Mo7O24: A Guanidinium Molybdate as a UV Nonlinear Optical Crystal with Large Birefringence171D Tin(II)‐Based Chiral Hybrid Perovskite Single Crystals with Extremely Distorted Inorganic Chains for Second Harmonic Generation38[C(NH2)3][B(C2O2H4)2]: An Organic–Inorganic Hybrid Borate Containing Nonlinear-Optical Active Unit [B(C2O2H4)2]− with Solar-Blind-Region Optical Nonlinearity16Hg4(Te2O5)(SO4): A Giant Birefringent Sulfate Crystal Triggered by a Highly Selective Cation153Layered (C5H6ON)2[Sb2O(C2O4)3] with a large birefringence derived from the uniform arrangement of π-conjugated units11Giant ab‐Plane Birefringence in Quasi‐1D Fibrous Red Phosphorus13Giant ab‐Plane Birefringence in Quasi‐1D Fibrous Red Phosphorus0(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 Systems5Two Short-Wave UV Beryllium Selenites Exhibiting Diverse Optical Properties Stemming from Functional Group Arrangements8Enhanced 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 Construction116[C(NH2)3]10(MoO3)10(PO4)2(HPO4)2·5H2O: Synergy effect of multiple functional units results in significant birefringence10Breaking Boundaries: Giant Ultraviolet Birefringence in Dimension‐Reduced Zn‐Based Crystals66Breaking Boundaries: Giant Ultraviolet Birefringence in Dimension‐Reduced Zn‐Based Crystals8Gradual Increase in Birefringence of Antimony Oxalates through Precise Tuning of the Sb3+/[C2O4]2– Ratio7NaK5La2(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)6Cs2Pb(CO3)2: a novel mixed-metal carbonate with rare Pb-C-O one-dimensional chain0Na2B6SO13 with unprecedented [B6SO13]∞ double chains and largest birefringence among borosulfates induced by the uniform arrangement of [B3O7] units19A novel sodium manganese fluorooxalate crystal Na2Mn2(C2O4)2.5F·2H2O: Synthesis, structure, optical and thermal properties2π-Lone pair synergy in (C7H4NO4)(IO3): Optimal balance among SHG, birefringence, and bandgap performance29From B 3 O 3 (OH) 3 to B 3 O 3 F 3 : Uncovering Series of New Functional Units Based on [BO 2 F] Beneficial for Deep‐Ultraviolet Birefringence1(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 implantation11SbO(OH)2(IO3): The First Polar Sb5+‐Iodate with a Strong Second‐Harmonic Generation Response and a Wide Bandgap8From HgGa2(SeO3)4 to Hg2Ga(SeO3)2F: The first HgI-based selenite birefringent crystal triggered by linear groups and fluoride ions29Birefringence Disparity Induced by Synergistic Effects of Stereochemically Active Lone Pairs19Hg4InS2Cl5: Achieving Giant Optical Anisotropy by Introducing Well‐Aligned Linear [Hg2S2] Units14“All-four-in-one”: a novel mercury tellurite–nitrate Hg 3 (TeO 3 )(Te 3 O 7 )(NO 3 ) 2 exhibiting exceptional optical anisotropy29(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(C 7 H 3 NO 4 ) 2 Sb 2 F 2 ·2H 2 O: a pyridine-based compound shows large optical anisotropy4Design of a high-performance infrared birefringent crystal Ba 4 HgP 2 Se 10 via a low-dimensional motif intercalation strategy2Four noncentrosymmetric molybdophosphates discovered by a chemical substitution strategy4Greatly enhancing birefringence of fluorosilicates through the synergetic effect of functional units13

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  4. An organic–inorganic hybrid birefringent material with diverse functional groups

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  5. Barium fluoroiodate crystals with a large band gap and birefringence

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  13. Sn2PO4I: An Excellent Birefringent Material with Giant Optical Anisotropy in Non π‐Conjugated Phosphate

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  17. Helical {[HgS]} n Chain-Induced Balanced Nonlinear-Optical Performance for Trigonal Mercury Sulfide

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  22. Ba 2 Zn 2 B 6 O 13 : coplanar [B 2 O 5 ] in unnoted U-shaped [B 6 O 13 ] groups achieving large birefringence

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  23. 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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  24. Hg 2 (SeO 3 )(SO 4 ): the first sulfate selenite with large birefringence explored from d 10 transition metal compounds

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  25. KSb(BeF 3 )F 3 : a totally fluorine strategy for achieving wide bandgap and large birefringence

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  26. Large optical anisotropy differentiation induced by the anion-directed regulation of structures

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  27. LiSrSbS 3 : parallel configurations of lone pair electrons inducing a large birefringence

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  28. Na 4 Ga 8 S 14 : a Ga-enriched wide band gap ternary alkali-metal sulfide with unique [Ga 12 S 42 ] 12-membered rings

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  30. Sn 9O 4Br 9X (X = Cl, Br): Two New Sn(II) Oxyhalides Exhibiting Large Birefringence Derived from Highly Distortive Polyhedra of Lone Pair Cations

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

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  33. From Pb(H 2 C 3 N 3 O 3 )(OH) to Pb(H 2 C 3 N 3 O 3 )F: Homovalent Anion Substitution-Induced Band Gap Enlargement and Birefringence Enhancement

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  35. First-principles study of the influence of lone pair electrons and molecular groups on the birefringence of phosphate and fluorophosphate

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  36. Potential optical functional crystals with large birefringence: Recent advances and future prospects

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  37. Explorations of New SHG Materials in Mercury Iodate Sulfate System**

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  38. Two Indium Iodate–Nitrates with Large Birefringence Induced by Hybrid Anionic Functional Groups and Their Favorable Arrangements

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  39. Layered Perovskite-like Nitrate Cs2Pb(NO3)2Br2 as a Multifunctional Optical Material

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  40. Promising Deep‐Ultraviolet Birefringent Materials via Rational Design and Assembly of Planar π‐Conjugated [B(OH)3] and [B3O3(OH)3] Functional Species

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  41. Promising Deep‐Ultraviolet Birefringent Materials via Rational Design and Assembly of Planar π‐Conjugated [B(OH)3] and [B3O3(OH)3] Functional Species

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  42. Realization of Enlarged Birefringence from BaCdBe2(BO3)2F2 to NaMgBe2(BO3)2F via the Cation Size Effect as a Potential Deep-Ultraviolet Birefringent Material

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  43. NaBaBS3: A Promising Infrared Functional Material with Large Birefringence Induced by π-Conjugated [BS3] Units

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  44. Pressure induced modulations in the optoelectronic properties of Hg2Cl2 compound: Insights from the first-principle calculations

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  45. A new birefringent material, HfF2(IO3)2, with a large birefringence and improved overall performances achieved by the integration of functional groups

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  46. ZrF2(IO3)2 and RbGaF3(IO3): Two Promising Birefringent Crystals Featuring 1D Metal-Fluoride Cationic Chains and Wide Bandgaps

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  47. Sn3B10O17Cl2 Achieving Birefringence Enhancement by Stereochemical Activity Lone Pair

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  48. Li2PbB2O5: A Pyroborate with Large Birefringence Induced by the Synergistic Effect of Stereochemical Active Lone Pair Cations and π-Conjugated [B2O5] Groups

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  49. LiKCuP2O7: Cation substitution application with mixed-alkaline copper-containing pyrophosphate and magnetic properties

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  50. Rb 3 B 5 O 8 F 2 and K 0.6 Rb 2.4 B 5 O 8 F 2 : two new deep-ultraviolet transparent nonlinear optical fluorooxoborates designed by cation regulation

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