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RESEARCH PAPER · Angewandte Chemie · 2016

Pb2BO3Cl: A Tailor‐Made Polar Lead Borate Chloride with Very Strong Second Harmonic Generation

Guohong Zou, Chensheng Lin, Hongil Jo, Gnu Nam, Tae‐Soo You, Kang Min Ok

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Pb2BO3Cl: A Tailor‐Made Polar Lead Borate Chloride with Very Strong Second Harmonic GenerationOriginalExperimental and ab initio studies of two UV nonlinear optical materials15ScMO(BO 3 ) (M = Ca and Cd): new Sc-based oxyborates featuring interesting edge-sharing sandwich-like chains and UV cut-off edges17The first quaternary diamond-like semiconductor with 10-membered LiS 4 rings exhibiting excellent nonlinear optical performances104Thioborates: potential nonlinear optical materials with rich structural chemistry51Bi3OF3(IO3)4: Metal Oxyiodate Fluoride Featuring a Carbon-Nanotube-like Topological Structure with Large Second Harmonic Generation Response121Studies on nonlinear optical ammonium pentaborate crystals27Design and Synthesis of a Series of Novel Mixed Borate and Carbonate Halides21CsB 4 O 6 F: A Congruent‐Melting Deep‐Ultraviolet Nonlinear Optical Material by Combining Superior Functional Units184CsB4O6F: A Congruent‐Melting Deep‐Ultraviolet Nonlinear Optical Material by Combining Superior Functional Units895LiGaGe2S6: A Chalcogenide with Good Infrared Nonlinear Optical Performance and Low Melting Point56Design and synthesis of a nonlinear optical material BaAl 4 S 7 with a wide band gap inspired from SrB 4 O 763Ion-induced structural and optical performance evolution in LBO-like crystals: experimental and theoretical investigation13NaBaM III Q 3 (M III = Al, Ga; Q = S, Se): first quaternary chalcogenides with isolated edge-sharing (MIII2Q 6 ) 6− dimers8Remarkable multimember-ring configurations in a new family of Na 7 M II Sb 5 S 12 (M II = Zn, Cd, Hg) exhibiting various three-dimensional tunnel structures25Cation‐Tuned Synthesis of Fluorooxoborates: Towards Optimal Deep‐Ultraviolet Nonlinear Optical Materials191Cation‐Tuned Synthesis of Fluorooxoborates: Towards Optimal Deep‐Ultraviolet Nonlinear Optical Materials714New silicate-germanate Cs2Pb2[(Si0.6Ge0.4)2O7] from the series A2Pb2[B2O7], A = K, Cs, B = Si, Ge with the umbrella-like [PbO3]4- group9SrB 5 O 7 F 3 Functionalized with [B 5 O 9 F 3 ] 6− Chromophores: Accelerating the Rational Design of Deep‐Ultraviolet Nonlinear Optical Materials738SrB5O7F3 Functionalized with [B5O9F3]6− Chromophores: Accelerating the Rational Design of Deep‐Ultraviolet Nonlinear Optical Materials116Computer-Assisted Design of a Superior Be 2 BO 3 F Deep-Ultraviolet Nonlinear-Optical Material41Rb 3 VO(O 2 ) 2 CO 3 : A Four‐in‐One Carbonatoperoxovanadate Exhibiting an Extremely Strong Second‐Harmonic Generation Response207Rb3VO(O2)2CO3: A Four‐in‐One Carbonatoperoxovanadate Exhibiting an Extremely Strong Second‐Harmonic Generation Response42Combination of d 10 -cations and fluorine anion as active participants to design novel borate/carbonate nonlinear optical materials24From LiB3O5 to NaRbB6O9F2: Fluorine‐Directed Evolution of Structural Chemistry33Synthesis and Characterization of the First Tin Fluoride Borate Sn3[B3O7]F with Second Harmonic Generation Response28The First Examples of Lithium‐Containing Mixed‐Alkali Strontium Borates with Different Dimensional Anionic Architectures and Short Cutoff Edges16Li2BaSc(BO3)2F and LiBa2Pb(BO3)2F with Layered Structures featuring Special Li−O/F Configurations11BaB2S4: An Efficient and Air-Stable Thioborate as Infrared Nonlinear Optical Material with High Laser Damage Threshold85Two Lanthanide Borate Chlorides LnB4O6(OH)2Cl (Ln = La, Ce) with Wide Ultraviolet Transmission Windows and Large Second-Harmonic Generation Responses25Y2(CO3)3·H2O and (NH4)2Ca2Y4(CO3)9·H2O: Partial Aliovalent Cation Substitution Enabling Evolution from Centrosymmetry to Noncentrosymmetry for Nonlinear Optical Response37Li 4 Na 2 CsB 7 O 14 : a new edge-sharing [BO 4 ] 5− tetrahedra containing borate with high anisotropic thermal expansion52ABaSbQ 3 (A = Li, Na; Q = S, Se): diverse arrangement modes of isolated SbQ 3 ligands regulating the magnitudes of birefringences50Ba 3 Ca 4 (BO 3 ) 3 (SiO 4 )Cl: a new non-centrosymmetric complex alkaline-earth metal borosilicate chloride with a deep-ultraviolet cut-off edge19Pb 2 Cd(SeO 3 ) 2 X 2 (X = Cl and Br): two halogenated selenites with phase matchable second harmonic generation27Sn 2 B 7 O 12 F with a 2∞[B 14 O 24 ] 6− layer constructed from the unprecedented [B 7 O 16 ] 11− fundamental building block18The effect of adding zinc sulphide nano-particles on structural, functional, thermal, dielectric, impedance and nonlinear optical properties of ammonium pentaborate crystals11KLi(HC 3 N 3 O 3 )·2H 2 O: Solvent-drop Grinding Method toward the Hydro-isocyanurate Nonlinear Optical Crystal314CsSbF 2 SO 4 : An Excellent Ultraviolet Nonlinear Optical Sulfate with a KTiOPO 4 (KTP)‐type Structure87CsSbF2SO4: An Excellent Ultraviolet Nonlinear Optical Sulfate with a KTiOPO4 (KTP)‐type Structure432[Ge2S5(S2)]4−, A NLO‐Active Unit Leading to an Asymmetric Structure Discovered in Li2Cs4Ge2S5(S2)Cl2: An Experimental and Theoretical study18BaB 2 O 3 F 2 : A Barium Fluorooxoborate with a Unique [B 2 O 3 F] − Layer and Short Cutoff Edge38Deep-Ultraviolet Mixed-Alkali-Metal Borates with Induced Enlarged Birefringence Derived from the Structure Rearrangement of the LiB3O545Dislocations that Decrease Size Mismatch within the Lattice Leading to Ultrawide Band Gap, Large Second‐Order Susceptibility, and High Nonlinear Optical Performance of AgGaS229Dislocations that Decrease Size Mismatch within the Lattice Leading to Ultrawide Band Gap, Large Second‐Order Susceptibility, and High Nonlinear Optical Performance of AgGaS2186β‐CsB9O14: A Triple‐Layered Borate with Edge‐Sharing BO4 Tetrahedra Exhibiting a Short Cutoff Edge and a Large Birefringence30K5B19O31: A Deep‐Ultraviolet Congruent Melting Compound6Sn2B5O9Cl: A Material with Large Birefringence Enhancement Activated Prepared via Alkaline‐Earth‐Metal Substitution by Tin255Sn2B5O9Cl: A Material with Large Birefringence Enhancement Activated Prepared via Alkaline‐Earth‐Metal Substitution by Tin33RbNa(HC 3 N 3 O 3 )·2H 2 O exhibiting a strong second harmonic generation response and large birefringence as a new potential UV nonlinear optical material69Emergent Deep‐Ultraviolet Nonlinear Optical Candidates324Neue Kandidaten für die nichtlineare Optik im Tief‐UV‐Bereich43A Promising Fluorooxoborate Framework with Flexibile Capability for Diverse Cations to Enhance the Second Harmonic Generation14An Unprecedented Antimony(III) Borate with Strong Linear and Nonlinear Optical Responses224An Unprecedented Antimony(III) Borate with Strong Linear and Nonlinear Optical Responses42Synthesis, Crystal Structure, and Characterization of a Noncentrosymmetric Sulfate Cs2Ca2(SO4)320Lead Mixed Oxyhalides Satisfying All Fundamental Requirements for High‐Performance Mid‐Infrared Nonlinear Optical Materials164Lead Mixed Oxyhalides Satisfying All Fundamental Requirements for High‐Performance Mid‐Infrared Nonlinear Optical Materials55Two Pyrophosphates with Large Birefringences and Second‐Harmonic Responses as Ultraviolet Nonlinear Optical Materials137Two Pyrophosphates with Large Birefringences and Second‐Harmonic Responses as Ultraviolet Nonlinear Optical Materials29CsHgNO3Cl2: A New Nitrate UV Birefringent Material Exhibiting an Optimized Layered Structure49Pb 18 O 8 Cl 15 I 5 : A Polar Lead Mixed Oxyhalide with Unprecedented Architecture and Excellent Infrared Nonlinear Optical Properties165Pb18O8Cl15I5: A Polar Lead Mixed Oxyhalide with Unprecedented Architecture and Excellent Infrared Nonlinear Optical Properties29Recent Advances in Oxide‐based Nonlinear Optical Materials with Wide Infrared Transparency Beyond 6 μm38Ba3(BO3)(CO3)F: The First Borate Carbonate Fluoride Synthesized by the High‐Temperature Solution Method19Series of Crystals with Giant Optical Anisotropy: A Targeted Strategic Research19Series of Crystals with Giant Optical Anisotropy: A Targeted Strategic Research140Cs 3 Pb 2 (CH 3 COO) 2 X 5 (X=I, Br): Halides with Strong Second‐Harmonic Generation Response Induced by Acetate Groups75Cs3Pb2(CH3COO)2X5 (X=I, Br): Halides with Strong Second‐Harmonic Generation Response Induced by Acetate Groups22Giant Optical Anisotropy in the UV‐Transparent 2D Nonlinear Optical Material Sc(IO 3 ) 2 (NO 3 )212Giant Optical Anisotropy in the UV‐Transparent 2D Nonlinear Optical Material Sc(IO 3 ) 2 (NO 3 )57α‐SnF 2 : A UV Birefringent Material with Large Birefringence and Easy Crystal Growth24α‐SnF 2 : A UV Birefringent Material with Large Birefringence and Easy Crystal Growth210Sn 14 O 11 Br 6 : a promising birefringent material with a [Sn 14 O 11 Br 6 ] layer26New Polymorphism for Ba3Zn2(BO3)3F with Two Polymorphs Exhibiting Anomalous Phase Transition2M3B6O10NO3 (M = K, Rb): Two New Alkali Metal Borate‐Nitrates with Noncentrosymmetric Structures20Discovery of First Magnesium Fluorooxoborate with Stable Fluorine Terminated Framework for Deep‐UV Nonlinear Optical Application167Discovery of First Magnesium Fluorooxoborate with Stable Fluorine Terminated Framework for Deep‐UV Nonlinear Optical Application18Cs4B4O3F10: First Fluorooxoborate with [BF4] Involving Heteroanionic Units and Extremely Low Melting Point18Be2(BO3)(IO3): The First Anion‐mixed Van der Waals Member in the KBe2BO3F2 Family with a Very Strong Second Harmonic Generation Response130Be2(BO3)(IO3): The First Anion‐mixed Van der Waals Member in the KBe2BO3F2 Family with a Very Strong Second Harmonic Generation Response8KCs2[Pb2Br5(HCOO)2]: A Polar 3D Lead‐Bromide Framework Exhibiting Strong Second‐Harmonic Generation Response10[Ag(NH 3 ) 2 ] 2 SO 4 : A Strategy for the Coordination of Cationic Moieties to Design Nonlinear Optical Materials**6[Ag(NH3)2]2SO4: A Strategy for the Coordination of Cationic Moieties to Design Nonlinear Optical Materials**85Sn2PO4I: 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 Phosphate22An Effective Strategy for Designing Nonlinear Optical Crystals by Combining the Structure‐Directing Property of Oxyfluorides with Chemical Substitution73An Effective Strategy for Designing Nonlinear Optical Crystals by Combining the Structure‐Directing Property of Oxyfluorides with Chemical Substitution10Strong SHG Responses in a Beryllium‐Free Deep‐UV‐Transparent Hydroxyborate via Covalent Bond Modification89Strong SHG Responses in a Beryllium‐Free Deep‐UV‐Transparent Hydroxyborate via Covalent Bond Modification9From β‐Na2B6O10 to Na3AlB8O15 and Na3Al2B7O15: Structural Tuning of Anionic‐Group Architectures by Substitution of [BO4] by [AlO4] Covalent Tetrahedra10A Lanthanum Ammonium Sulfate Double Salt with a Strong SHG Response and Wide Deep‐UV Transparency15A Lanthanum Ammonium Sulfate Double Salt with a Strong SHG Response and Wide Deep‐UV Transparency96( R )- and ( S )-[C 8 H 10 NO 3 ] 2 [NbOF 5 ]: noncentrosymmetric niobium oxyfluorides with large optical anisotropy3Ba 10 LuB 18 O 32 F 13 : the first example of borate in the Lu–B–O–F system with the unprecedented FBB [B 9 O 22 ]12KPb 3 ( o -C 5 H 4 NCOO) 2 Cl 5 : a brand-new stable lead chloride with good comprehensive nonlinear optical performance5Large optical anisotropy differentiation induced by the anion-directed regulation of structures29PNO: a promising deep-UV nonlinear optical material with the largest second harmonic generation effect17Three-dimensional all-inorganic dual halogen emitter Cs 2 Cd 2 BrCl 5 exhibiting broadband white-light emission18Chiral Ligand‐Driven Systematic Synthesis of Coordination Polymers with Non‐centrosymmetric Structures12Introducing a New d0 Sc3+ Asymmetric Ion for Functional Materials: Large Birefringence Enhancement by ScO6 in Ba3Sc2(BO3)411Strong Nonlinearity Induced by Coaxial Alignment of Polar Chain and Dense [BO3] Units in CaZn2(BO3)212Strong Nonlinearity Induced by Coaxial Alignment of Polar Chain and Dense [BO3] Units in CaZn2(BO3)2212Corrugated 1D Hybrid Metal Halide [C6H7ClN]CdCl3 Exhibiting Broadband White-Light Emission46Realization of Enlarged Birefringence from BaCdBe2(BO3)2F2 to NaMgBe2(BO3)2F via the Cation Size Effect as a Potential Deep-Ultraviolet Birefringent Material18Double‐Modification Oriented Design of a Deep‐UV Birefringent Crystal Functionalized by [B12O16F4(OH)4] Clusters9Double‐Modification Oriented Design of a Deep‐UV Birefringent Crystal Functionalized by [B12O16F4(OH)4] Clusters139Hybrid Germanium Bromide Perovskites with Tunable Second Harmonic Generation122Hybrid Germanium Bromide Perovskites with Tunable Second Harmonic Generation8Perfectly Encoding π‐Conjugated Anions in the RE5(C3N3O3)(OH)12 (RE=Y, Yb, Lu) Family with Strong Second Harmonic Generation Response and Balanced Birefringence91Perfectly Encoding π‐Conjugated Anions in the RE5(C3N3O3)(OH)12 (RE=Y, Yb, Lu) Family with Strong Second Harmonic Generation Response and Balanced Birefringence18Recent Advances in Infrared Nonlinear Optical Crystal7Polar Phosphorus Chalcogenide Cage Molecules: Enhancement of Nonlinear Optical Properties in Adducts38Polar Phosphorus Chalcogenide Cage Molecules: Enhancement of Nonlinear Optical Properties in Adducts1The First UV Nonlinear Optical Selenite Material: Fluorination Control in CaYF(SeO 3 ) 2 and Y 3 F(SeO 3 ) 485The First UV Nonlinear Optical Selenite Material: Fluorination Control in CaYF(SeO3)2 and Y3F(SeO3)47Efficient Synthesis, Spectroscopic Characterization, and Nonlinear Optical Properties of Novel Salicylaldehyde-Based Thiosemicarbazones: Experimental and Theoretical Studies37Cd2Nb2Te4O15: A Novel Pseudo‐Aurivillius‐Type Tellurite with Unprecedented Nonlinear Optical Properties and Excellent Stability40Pb3[O10Pb20](SiO4)4X10 (X = Cl, Br): The First Pb-Containing Halogen Silicates with Mirror-Symmetric Pseudo-Aurivillius Bilayers3[C3H7N6]3[B3O5(OH)2] and [C3H8N6]4[B12O19(OH)6]: Two Melamine Borates with Large Birefringence13Ba 3 Al 2 B 12 O 24 : a beryllium-free member of the Sr 2 Be 2 B 2 O 7 family with a 2 ∞ [B 12 Al 2 O 28 ] double-layered structure4(NH 4 ) 2 Cd 2 Cl 3 F 3 and (NH 4 ) 2 Cd 2 Br 3 F 3 : The First Fluoride‐Containing d 10 Metal Mixed Halides Exhibiting Superior Ultraviolet Nonlinear Optical Properties28Designing High-Performance Short-Wave UV Tellurium-Based Mixed Halides Birefringent Crystals via Halogen Substitution Engineering4Strongly Polar [H2PO3]− Induced π-Conjugated Group Arrangement for Balanced UV Nonlinear Optical Performance3Out-of-Plane Polarization in a 2D Ruddlesden–Popper Hybrid Lead Halide Perovskite Ferroelectric Semiconductor7Recent Progress in the Design and Synthesis of Nonlinear Optical Crystals with Stereochemically Active Lone Pairs8Achieving record-high birefringence in a 3D fluorozincoborate via coplanar alignment of π-conjugated [BO 3 ] units0Exploring the Effect of Electronic Symmetry on the Hyperpolarizabilities of Co(II) and Ni(II) Coordination Complexes with Cytidine Nucleotide6Electronegativity Adaption Approach for Solar‐Blind UV Birefringent Crystals With Ultrawide Bandgaps1Positional Isomerism Controls Polarity and Nonlinear Optical Properties in One‐Dimensional Hybrid Germanium Halides0

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  2. ScMO(BO 3 ) (M = Ca and Cd): new Sc-based oxyborates featuring interesting edge-sharing sandwich-like chains and UV cut-off edges

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  4. Thioborates: potential nonlinear optical materials with rich structural chemistry

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  5. Bi3OF3(IO3)4: Metal Oxyiodate Fluoride Featuring a Carbon-Nanotube-like Topological Structure with Large Second Harmonic Generation Response

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  6. Studies on nonlinear optical ammonium pentaborate crystals

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  8. CsB 4 O 6 F: A Congruent‐Melting Deep‐Ultraviolet Nonlinear Optical Material by Combining Superior Functional Units

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  9. CsB4O6F: A Congruent‐Melting Deep‐Ultraviolet Nonlinear Optical Material by Combining Superior Functional Units

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  10. LiGaGe2S6: A Chalcogenide with Good Infrared Nonlinear Optical Performance and Low Melting Point

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  11. Design and synthesis of a nonlinear optical material BaAl 4 S 7 with a wide band gap inspired from SrB 4 O 7

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  13. NaBaM III Q 3 (M III = Al, Ga; Q = S, Se): first quaternary chalcogenides with isolated edge-sharing (MIII2Q 6 ) 6− dimers

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  14. Remarkable multimember-ring configurations in a new family of Na 7 M II Sb 5 S 12 (M II = Zn, Cd, Hg) exhibiting various three-dimensional tunnel structures

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  17. New silicate-germanate Cs2Pb2[(Si0.6Ge0.4)2O7] from the series A2Pb2[B2O7], A = K, Cs, B = Si, Ge with the umbrella-like [PbO3]4- group

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  23. Combination of d 10 -cations and fluorine anion as active participants to design novel borate/carbonate nonlinear optical materials

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  29. Two Lanthanide Borate Chlorides LnB4O6(OH)2Cl (Ln = La, Ce) with Wide Ultraviolet Transmission Windows and Large Second-Harmonic Generation Responses

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  30. Y2(CO3)3·H2O and (NH4)2Ca2Y4(CO3)9·H2O: Partial Aliovalent Cation Substitution Enabling Evolution from Centrosymmetry to Noncentrosymmetry for Nonlinear Optical Response

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  31. Li 4 Na 2 CsB 7 O 14 : a new edge-sharing [BO 4 ] 5− tetrahedra containing borate with high anisotropic thermal expansion

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  32. ABaSbQ 3 (A = Li, Na; Q = S, Se): diverse arrangement modes of isolated SbQ 3 ligands regulating the magnitudes of birefringences

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  33. Ba 3 Ca 4 (BO 3 ) 3 (SiO 4 )Cl: a new non-centrosymmetric complex alkaline-earth metal borosilicate chloride with a deep-ultraviolet cut-off edge

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  34. Pb 2 Cd(SeO 3 ) 2 X 2 (X = Cl and Br): two halogenated selenites with phase matchable second harmonic generation

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  35. Sn 2 B 7 O 12 F with a 2∞[B 14 O 24 ] 6− layer constructed from the unprecedented [B 7 O 16 ] 11− fundamental building block

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  36. The effect of adding zinc sulphide nano-particles on structural, functional, thermal, dielectric, impedance and nonlinear optical properties of ammonium pentaborate crystals

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  37. KLi(HC 3 N 3 O 3 )·2H 2 O: Solvent-drop Grinding Method toward the Hydro-isocyanurate Nonlinear Optical Crystal

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  38. CsSbF 2 SO 4 : An Excellent Ultraviolet Nonlinear Optical Sulfate with a KTiOPO 4 (KTP)‐type Structure

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  39. CsSbF2SO4: An Excellent Ultraviolet Nonlinear Optical Sulfate with a KTiOPO4 (KTP)‐type Structure

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  40. [Ge2S5(S2)]4−, A NLO‐Active Unit Leading to an Asymmetric Structure Discovered in Li2Cs4Ge2S5(S2)Cl2: An Experimental and Theoretical study

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