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RESEARCH PAPER · Angewandte Chemie International Edition · 2018

NH4Be2BO3F2 and γ‐Be2BO3F: Overcoming the Layering Habit in KBe2BO3F2 for the Next‐Generation Deep‐Ultraviolet Nonlinear Optical Materials

Guang Peng, Ning Ye, Zheshuai Lin, Lei Kang, Shilie Pan, Min Zhang, Chensheng Lin, Xifa Long, Min Luo, Yu Chen, Yu‐Huan Tang, Feng Xu, Tao Yan

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NH4Be2BO3F2 and γ‐Be2BO3F: Overcoming the Layering Habit in KBe2BO3F2 for the Next‐Generation Deep‐Ultraviolet Nonlinear Optical MaterialsOriginalFluorooxoborates: Ushering in a New Era of Deep Ultraviolet Nonlinear Optical Materials102The Rubidium Barium Borate Resulting from B7O15 Fundamental Building Block Exhibits DUV Cutoff Edge17The linear and nonlinear optical response of CsGeX3 (X=Cl, Br, and I): The finite field and first-principles investigation26Cyano-Based Materials with Giant Optical Anisotropy and Second Harmonic-Generation Effect24BaPO3Cl: a Metal Phosphate Chloride with Infinite [PO3]∞ Chains25Y2(CO3)3·H2O and (NH4)2Ca2Y4(CO3)9·H2O: Partial Aliovalent Cation Substitution Enabling Evolution from Centrosymmetry to Noncentrosymmetry for Nonlinear Optical Response37A Facile Route to Nonlinear Optical Materials: Three‐Site Aliovalent Substitution Involving One Cation and Two Anions137A Facile Route to Nonlinear Optical Materials: Three‐Site Aliovalent Substitution Involving One Cation and Two Anions23Growth, Crystal Structures, and Characteristics of Li 5 ASrMB 12 O 24 (A = Zn, Mg; M = Al, Ga) with [MB 12 O 24 ] Frameworks12A 2 Bi 2 (SO 4 ) 2 Cl 4 (A = NH 4 , K, Rb): achieving a subtle balance of the large second harmonic generation effect and sufficient birefringence in sulfate nonlinear optical materials98Ba 3 B 10 O 17 F 2 ·0.1KF: the first mixed alkali/alkaline-earth metal fluorooxoborate with unprecedented double-layered B–O/F anionic arrangement17Hybridization-activated new deep ultraviolet transparent nonlinear optical material Ba 11 [Al(PO 4 ) 4 ](P 2 O 7 )(PO 4 ) 3 with balanced overall performance and parsimony-forbidden structure23K 2 SrP 4 O 12 : a deep-UV transparent cyclophosphate as a nonlinear optical crystal79Pb 10 O 4 (BO 3 ) 3 I 3 : a new noncentrosymmetric oxyborate iodide synthesized by the straightforward hydrothermal method6RE(H 2 C 3 N 3 O 3 ) 2 ·(OH)· x H 2 O (RE = La, Y and Gd): potential UV birefringent materials with strong optical anisotropy originating from the (H 2 C 3 N 3 O 3 ) − group31Sr[B(OH) 4 ](IO 3 ) and Li 4 Sr 5 [B 12 O 22 (OH) 4 ](IO 3 ) 2 : two unprecedented metal borate-iodates showing a subtle balance of enlarged band gap and birefringence34Structural insights into three phosphates with distinct polyanionic configurations20The first lithium difluorophosphate LiPO 2 F 2 with a neutral polytetrahedral microporous architecture35Y 8 O(OH) 15 (CO 3 ) 3 Cl: an excellent short-wave UV nonlinear optical material exhibiting an infrequent three-dimensional inorganic cationic framework61Li2CsB7O10(OH)4: A Deep-Ultraviolet Nonlinear-Optical Mixed-Alkaline Borate Constructed by Unusual Heptaborate Anions98BeO6 Trigonal Prism with Ultralong Be–O Bonds Observed in a Deep Ultraviolet Optical Crystal Li13BeBe6B9O2712A New Cadmium‐Based Pb2Cd3(PO4)2(P2O7) with Two Types of Isolated P–O Groups18Zeolitic Open-Framework Borates with Noncentrosymmetric Structures and Nonlinear Optical Properties24Deep-ultraviolet nonlinear optical crystal NaBe2BO3F2—Structure, growth and optical properties25Ba10In6Zn7S10Se16 and Ba10In6Zn7Se26: Two new infrared nonlinear optical materials with T2 super tetrahedron6KNa 4 B 2 P 3 O 13 : A Deep-Ultraviolet Transparent Borophosphate Exhibiting Second-Harmonic Generation Response26Poly(difluorophosphazene) as the First Deep‐Ultraviolet Nonlinear Optical Polymer: A First‐Principles Prediction35Poly(difluorophosphazene) as the First Deep‐Ultraviolet Nonlinear Optical Polymer: A First‐Principles Prediction14Rb7SrY2(B5O10)3: A Rare-Earth Pentaborate with Moderate Second-Harmonic Response and Interesting Phase-Matching Behavior29Centrosymmetric Rb2Mg3(SO4)4 and non-centrosymmetric Cs2Mg3(SO4)4 with a phase-matching nonlinear optical response35Nitrate nonlinear optical crystals: A survey on structure-performance relationships146Nontoxic KBBF Family Member Zn2BO3(OH): Balance between Beneficial Layered Structure and Layer Tendency81LiMII(IO3)3 (MII=Zn and Cd): Two Promising Nonlinear Optical Crystals Derived from a Tunable Structure Model of α‐LiIO398LiMII(IO3)3 (MII=Zn and Cd): Two Promising Nonlinear Optical Crystals Derived from a Tunable Structure Model of α‐LiIO337First-Principles Design and Simulations Promote the Development of Nonlinear Optical Crystals299KMg(H 2 O)PO 4 : A Deep-Ultraviolet Transparent Nonlinear Optical Material Derived from KTiOPO 483A new iodate-phosphate Pb 2 (IO 3 )(PO 4 ) achieving great improvement in birefringence activated by (IO 3 ) − groups53An unprecedented planar π-conjugated [B 2 P 5 ] 5− group with ultra-large birefringence and nonlinearity: an ab initio study17(NH4)Bi2(IO3)2F5: An Unusual Ammonium‐Containing Metal Iodate Fluoride Showing Strong Second Harmonic Generation Response and Thermochromic Behavior92(NH4)Bi2(IO3)2F5: An Unusual Ammonium‐Containing Metal Iodate Fluoride Showing Strong Second Harmonic Generation Response and Thermochromic Behavior11Emergent Deep‐Ultraviolet Nonlinear Optical Candidates324Neue Kandidaten für die nichtlineare Optik im Tief‐UV‐Bereich43“Old dog, new tricks”: the lone pair effect inducing divergent optical responses in lead cyanurates containing π-bonds18Syntheses, characterization, and theoretical calculation of Rb2Mg3(P2O7)2 polymorphs with deep-ultraviolet cutoff edges18A series of Er3+-activated SrLaGa3O7 single crystal fibers for mid-infrared laser application18(NH 4 ) 3 [B(OH) 3 ] 2 (COOH) 3 : a graphite-like UV nonlinear optical material with a large birefringence via structural optimization312(C 3 H 7 N 6 ) + ·2Cl − ·H 2 O: an ultraviolet nonlinear optical crystal with large birefrigence and strong second-harmonic generation78Helix-constructed polar rare-earth iodate fluoride as a laser nonlinear optical multifunctional material25Hydroisocyanurates X 2 Y(H 2 C 3 N 3 O 3 ) 4 ·4H 2 O (X = K, Cs; Y = Zn, Cd) with large birefringence stemming from π-conjugated (H 2 C 3 N 3 O 3 ) − anions28Inorganic planar π-conjugated groups in nonlinear optical crystals: review and outlook145Na 3 Sc 2 (PO 4 ) 2 F 3 : rational design and synthesis of an alkali rare-earth phosphate fluoride as an ultraviolet nonlinear optical crystal with an enlarged birefringence49Prediction of ternary fluorooxoborates with coplanar triangular units [BO x F 3−x ] x− from first-principles13Two-stage evolution from phosphate to sulfate of new KTP-type family members as UV nonlinear optical materials through chemical cosubstitution-oriented design51Structure-property relationship in nonlinear optical materials with π-conjugated CO3 triangles146Synthesis, Crystal Structure, and Characterization of a Noncentrosymmetric Sulfate Cs2Ca2(SO4)320Two New Ferroborates with Three‐Dimensional Framework and Wide Transmittance Window2Enhanced nonlinear optical functionality in birefringence and refractive index dispersion of the deep-ultraviolet fluorooxoborates123Synthesis, characterizations and theoretical analysis of a noncentrosymmetric sulfate8Syntheses, characterization and calculations of LimAnM6O15 (A=Rb, Cs; M=Si, Ge; m+n=6)18A review on phase transition and structure-performance relationship of second-order nonlinear optical polymorphs107Deep-ultraviolet nonlinear optical crystals by design: A computer-aided modeling blueprint from first principles45Realizing Deep-Ultraviolet Second Harmonic Generation by First-Principles-Guided Materials Exploration in Hydroxyborates111The study of structure evolvement of KTiOPO4 family and their nonlinear optical properties98Sr5[BO2(OH)]3(OH)3F: First hydroxyborate fluoride with the [BO2(OH)]2− unit2Zn3B7O13Cl: A New Deep-Ultraviolet Transparency Nonlinear Optical Crystal with Boracite Structure24Anionic Aliovalent Substitution from Structure Models of ZnS: Novel Defect Diamond‐like Halopnictide Infrared Nonlinear Optical Materials with Wide Band Gaps and Large SHG Effects78Anionic Aliovalent Substitution from Structure Models of ZnS: Novel Defect Diamond‐like Halopnictide Infrared Nonlinear Optical Materials with Wide Band Gaps and Large SHG Effects19Ba 2 B 7 O 12 F with novel FBB [B 7 O 16 F] and deep-ultraviolet cut-off edge31Mechanochemical Synthesis of an Ionic Cocrystal with Large Birefringence Resulting from Neutral Planar π-Conjugated Groups26Layered oxide B2S2O9 with a deep-ultraviolet band gap and a strong and robust second-harmonic generation32NaZnCO 3 (OH): A High-Performance Carbonate Ultraviolet Nonlinear Optical Crystal Derived from KBe 2 BO 3 F 2194Borates: A Rich Source for Optical Materials1089Predicting Berborite as Potential Deep-Ultraviolet Nonlinear Optical Crystal from First Principles29Sb6O7(SO4)2: A Promising Ultraviolet Nonlinear Optical Material with an Enhanced Second‐Harmonic‐Generation Response Activated by SbIII Lone‐Pair Stereoactivity62Ba 3 [Al(PO 4 ) 3 ]: rational design of a promising deep-UV transparent SHG crystal with balanced overall performance originating from the condensation of quartz-type [Al(PO 4 ) 4 ] 9− units16A new acentric borate–nitrate Cs 3 B 8 O 13 (NO 3 ) with interpenetrating porous 3D covalent and ionic lattices8A new rare-earth borate birefringent crystal with quasi-two-dimensional [BO 3 ] layers23Ba 2 BS 3 Cl and Ba 5 B 2 S 8 Cl 2 : first alkaline-earth metal thioborate halides with [BS 3 ] units21Ba 4 Ca(B 2 O 5 ) 2 F 2 : π-conjugation of B 2 O 5 in the planar pentagonal layer achieving large second harmonic generation of pyro -borate34Computationally assisted multistage design and prediction driving the discovery of deep-ultraviolet nonlinear optical materials41Electro-optic modulation in a non-centrosymmetric antiferroelectric crystal2K 2 Pb(H 2 C 3 N 3 O 3 ) 4 (H 2 O) 4 : a potential UV nonlinear optical material with large birefringence50Recent advances of oxyfluorides for nonlinear optical applications69To improve the key properties of nonlinear optical crystals assembled with tetrahedral functional building units46Unexpected aliovalent cation substitution between two NLO materials LiBa 3 Bi 6 (SeO 3 ) 7 F 11 and Ba 3 Bi 6.5 (SeO 3 ) 7 F 10.5 O 0.518M(NH 2 SO 3 ) 2 (M=Sr, Ba): Two Deep‐Ultraviolet Transparent Sulfamates Exhibiting Strong Second Harmonic Generation Responses and Moderate Birefringence142M(NH 2 SO 3 ) 2 (M=Sr, Ba): Two Deep‐Ultraviolet Transparent Sulfamates Exhibiting Strong Second Harmonic Generation Responses and Moderate Birefringence27Large Second-Harmonic Response and Giant Birefringence of CeF 2 (SO 4 ) Induced by Highly Polarizable Polyhedra248Prediction of Novel van der Waals Boron Oxides with Superior Deep‐Ultraviolet Nonlinear Optical Performance43Prediction of Novel van der Waals Boron Oxides with Superior Deep‐Ultraviolet Nonlinear Optical Performance6Borosilicate Crystal LaBSiO5: A New Promising Ultraviolet Quasiphase Matching Material31Toward the Enhancement of Critical Performance for Deep-Ultraviolet Frequency-Doubling Crystals Utilizing Covalent Tetrahedra137Discovery 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 Application18Te(CS(NH2)2)4SO4·2H2O: A Three-in-One Semiorganic Nonlinear Optical Crystal with an Unusual Quadrilateral (TeS4)6– Chromophore14Expanding the chemistry of borates with functional [BO2]− anions200Deep‐Ultraviolet Nonlinear‐Optical van‐der‐Waals Beryllium Borates**6Struvite-type AMgPO4·6H2O (A = NH4, K): Two Natural Deep-Ultraviolet Transparent Nonlinear Optical Crystals13Fluorine‐Driven Enhancement of Birefringence in the Fluorooxosulfate: A Deep Evaluation from a Joint Experimental and Computational Study139LiB2O3F: A Beryllium-Free Deep-Ultraviolet Nonlinear Optical Material Designed Based on a Boron-Rich Strategy61Sr2Pb(BeB5O10)(BO3): An Excellent Ultraviolet Nonlinear-Optical Beryllium Borate by the Pb-Modified Construction of a Conjugated System and Lone-Pair Effect14A2MoO2F3(IO2F2) (A = Rb, Cs): Strong Nonlinear Optical Responses and Enlarged Band Gaps through Fluorine Incorporation50Exploring Deep-UV Nonlinear Optical Materials with Enhanced Second Harmonic Generation Response and Birefringence in Fluoroaluminoborate Crystals69Solvothermal Syntheses of Three-Dimensional Open-Framework Thioantimonates Displaying Nonlinear Optical Responses5A Congruent‐Melting Mid‐Infrared Nonlinear Optical Vanadate Exhibiting Strong Second‐Harmonic Generation22A Congruent‐Melting Mid‐Infrared Nonlinear Optical Vanadate Exhibiting Strong Second‐Harmonic Generation63Novel van der Waals Deep‐UV Nonlinear Optical Materials3A General Principle for DUV NLO Materials: π‐Conjugated Confinement Enlarges Band Gap**175A General Principle for DUV NLO Materials: π‐Conjugated Confinement Enlarges Band Gap**27Strong 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 Modification9Borate nonlinear optical single crystal surface finishing by argon cluster ion sputtering25Enhancement of band gap and birefringence induced via π -conjugated chromophore with “tail effect”28Designing A New Infrared Nonlinear Optical Material, β‐BaGa 2 Se 4 Inspired by the Phase Transition of the BaB 2 O 4 (BBO) Crystal75Designing A New Infrared Nonlinear Optical Material, β‐BaGa2Se4 Inspired by the Phase Transition of the BaB2O4 (BBO) Crystal13Structure and Origin of the Second-Harmonic Generation Response of Nonlinear Optical Material Sr2Be2B2O713From CeF2(SO4)·H2O to Ce(IO3)2(SO4): Defluorinated Homovalent Substitution for Strong Second-Harmonic-Generation Effect and Sufficient Birefringence53Sr 3 B 14 O 24 : a new borate with a [B 14 O 30 ] fundamental building block and an unwonted 2D double layer11Complex coordinated functional groups: A great genes for nonlinear optical materials64Hybrid organic–inorganic triguanidine arsenate dihydrate for ultraviolet nonlinear optical application15Na4B8O9F10: A Deep‐Ultraviolet Transparent Nonlinear Optical Fluorooxoborate with Unexpected Short Phase‐Matching Wavelength Induced by Optimized Chromatic Dispersion133Na4B8O9F10: A Deep‐Ultraviolet Transparent Nonlinear Optical Fluorooxoborate with Unexpected Short Phase‐Matching Wavelength Induced by Optimized Chromatic Dispersion13A 2 B 6 O 9 F 2 (A = NH 4 , K): new members of A 2 B 6 O 9 F 2 family with deep-UV cutoff edges and moderate birefringence17A flexible functional module to regulate ultraviolet optical nonlinearity for achieving a balance between a second-harmonic generation response and birefringence43K 2 (BeS)O 4 F 2 : a novel fluorosulfate with unprecedented 1D [(BeO 3 F)–(SO 3 F)] ∞ chains exhibiting large birefringence10Na 3 B 6 O 10 (HCOO): an ultraviolet nonlinear optical sodium borate-formate33Na 3 YB 8 O 15 : a new rare-earth borate with an infinite one-dimensional [B 8 O 15 ] ∞ chain and a short ultraviolet cutoff edge8Nain(C2o4)(Hpo4)(H2o)5: An Ultraviolet Transparent Nonlinear Optical Oxalate-Phosphate with Large Birefringence0PbBe 2 B 2 O 6 : an ultraviolet nonlinear-optical crystal with unprecedented π–π interacting BeBO 5 group13Wide bandgaps and strong SHG responses of hetero-oxyfluorides by dual-fluorination-directed bandgap engineering28Recent progress in the development of KBe2BO3F2: a deep-UV nonlinear optical crystal12Phosphogermanate Crystal: A New Ultraviolet–Infrared Nonlinear Optical Crystal with Excellent Optical Performances16Advances in second-order nonlinear optical sulfates38Sulfamide: A Promising Deep‐Ultraviolet Nonlinear Optical Crystal Assembled from Polar Covalent [SO2(NH2)2] Tetrahedra9Sulfamide: A Promising Deep‐Ultraviolet Nonlinear Optical Crystal Assembled from Polar Covalent [SO2(NH2)2] Tetrahedra84Inorganic nonlinear optical materials7Ba2B10O16(OH)2·(H3BO3)(H2O): A Possible Deep-Ultraviolet Nonlinear-Optical Barium Borate36First‐Principles Investigation About Different Sequence of Stereochemical Activity and Birefringence in Antimony Halides2Ultrawide Bandgap and Outstanding Second‐Harmonic Generation Response by a Fluorine‐Enrichment Strategy at a Transition‐Metal Oxyfluoride Nonlinear Optical Material51Ultrawide Bandgap and Outstanding Second‐Harmonic Generation Response by a Fluorine‐Enrichment Strategy at a Transition‐Metal Oxyfluoride Nonlinear Optical Material12A2BeS2O8 (A = NH4, K, Rb, Cs) Deep Ultraviolet Nonlinear Optical Crystals33Screening Nitrides with High Debye Temperatures as Nonlinear Optical Materials19Crystal Growth and Physical Properties of the Nonlinear Optical Crystal KLi(HC3N3O3)·2H2O15Alkali metal sulfate: A new non-π-conjugated deep-ultraviolet quasi-phase matching crystal27An Optimized KBe2BO3F2‐Like Structure: The Unity of Deep‐Ultraviolet Transparency, Nonlinear Optical Property, and Ferroelectricity22Double‐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] Clusters139Noncentrosymmetric (C3H7N6)6(H2PO4)4(HPO4)·4H2O and Centrosymmetric (C3H7N6)2SO4·2H2O: Exploration of Acentric Structure by Combining Planar and Tetrahedral Motifs via Hydrogen Bonds37Deep-ultraviolet nonlinear optical crystals: concept development and materials discovery181An excellent deep-ultraviolet birefringent material based on [BO2]∞ infinite chains185

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  5. BaPO3Cl: a Metal Phosphate Chloride with Infinite [PO3]∞ Chains

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  35. First-Principles Design and Simulations Promote the Development of Nonlinear Optical Crystals

    Accounts of Chemical Research · 2019-10-29

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  36. KMg(H 2 O)PO 4 : A Deep-Ultraviolet Transparent Nonlinear Optical Material Derived from KTiOPO 4

    Chemistry of Materials · 2019-11-01

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  37. A new iodate-phosphate Pb 2 (IO 3 )(PO 4 ) achieving great improvement in birefringence activated by (IO 3 ) − groups

    Chemical Communications · 2019-12-04

    Xiaohan Zhang, Bing‐Ping Yang, Jin Chen, Chun‐Li Hu, Zhi Gang Fang, Zujian Wang, Jiang‐Gao Mao

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  38. An unprecedented planar π-conjugated [B 2 P 5 ] 5− group with ultra-large birefringence and nonlinearity: an ab initio study

    Chemical Communications · 2019-12-04

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  39. (NH4)Bi2(IO3)2F5: An Unusual Ammonium‐Containing Metal Iodate Fluoride Showing Strong Second Harmonic Generation Response and Thermochromic Behavior

    Angewandte Chemie International Edition · 2019-12-09

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  40. (NH4)Bi2(IO3)2F5: An Unusual Ammonium‐Containing Metal Iodate Fluoride Showing Strong Second Harmonic Generation Response and Thermochromic Behavior

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  41. Emergent Deep‐Ultraviolet Nonlinear Optical Candidates

    Angewandte Chemie International Edition · 2019-12-10

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  42. Neue Kandidaten für die nichtlineare Optik im Tief‐UV‐Bereich

    Angewandte Chemie · 2019-12-10

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  43. “Old dog, new tricks”: the lone pair effect inducing divergent optical responses in lead cyanurates containing π-bonds

    Dalton Transactions · 2019-12-11

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  44. Syntheses, characterization, and theoretical calculation of Rb2Mg3(P2O7)2 polymorphs with deep-ultraviolet cutoff edges

    Science China Materials · 2019-12-20

    Hongping Wu, Shiwei Liu, Shichao Cheng, Hongwei Yu, Zhanggui Hu, Jiyang Wang, Yicheng Wu

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  45. A series of Er3+-activated SrLaGa3O7 single crystal fibers for mid-infrared laser application

    Journal of Rare Earths · 2019-12-27

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  46. (NH 4 ) 3 [B(OH) 3 ] 2 (COOH) 3 : a graphite-like UV nonlinear optical material with a large birefringence via structural optimization

    Chemical Communications · 2020-01-01

    Yalan Deng, Lei Wang, Yuwei Ge, Ling Huang, Daojiang Gao, Jian Bi, Guohong Zou

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  47. 2(C 3 H 7 N 6 ) + ·2Cl − ·H 2 O: an ultraviolet nonlinear optical crystal with large birefrigence and strong second-harmonic generation

    Chemical Communications · 2020-01-01

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  48. Helix-constructed polar rare-earth iodate fluoride as a laser nonlinear optical multifunctional material

    Chemical Science · 2020-01-01

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    CrystEngComm · 2020-01-01

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  50. Inorganic planar π-conjugated groups in nonlinear optical crystals: review and outlook

    Inorganic Chemistry Frontiers · 2020-01-01

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