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RESEARCH PAPER · Angewandte Chemie International Edition · 2018

Cation‐Tuned Synthesis of Fluorooxoborates: Towards Optimal Deep‐Ultraviolet Nonlinear Optical Materials

Ying Wang, Bingbing Zhang, Zhihua Yang, Shilie Pan

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Cation‐Tuned Synthesis of Fluorooxoborates: Towards Optimal Deep‐Ultraviolet Nonlinear Optical MaterialsOriginalCation-tuned synthesis of the A 2 SO 4 ·SbF 3 (A = Na + , NH 4 + , K + , Rb + ) family with nonlinear optical properties78Cs 3 VO(O 2 ) 2 CO 3 : an exceptionally thermostable carbonatoperoxovanadate with an extremely large second-harmonic generation response129Design of novel graphdiyne-based materials with large second-order nonlinear optical properties90Perfect balance harmony in Ba 2 NO 3 (OH) 3 : a beryllium-free nitrate as a UV nonlinear optical material184Pushing Nonlinear Optical Oxides into the Mid-Infrared Spectral Region Beyond 10 μm: Design, Synthesis, and Characterization of La3SnGa5O14145Pb2BO3I: A Borate Iodide with the Largest Second‐Harmonic Generation (SHG) Response in the KBe2BO3F2 (KBBF) Family of Nonlinear Optical (NLO) Materials237A Series of Rare-Earth Borates K 7 MRE 2 B 15 O 30 (M = Zn, Cd, Pb; RE = Sc, Y, Gd, Lu) with Large Second Harmonic Generation Responses103M2B10O14F6 (M = Ca, Sr): Two Noncentrosymmetric Alkaline Earth Fluorooxoborates as Promising Next-Generation Deep-Ultraviolet Nonlinear Optical Materials356Deep‐Ultraviolet Nonlinear Optical Crystal Cs2Al2(B3O6)2O: A Benign Member of the Sr2Be2(BO3)2O Family with [Al2(B3O6)2O]2− Double Layers70Polar Fluorooxoborate, NaB4O6F: A Promising Material for Ionic Conduction and Nonlinear Optics494Polar Fluorooxoborate, NaB4O6F: A Promising Material for Ionic Conduction and Nonlinear Optics67Rational Design of the First Lead/Tin Fluorooxoborates MB2O3F2 (M = Pb, Sn), Containing Flexible Two-Dimensional [B6O12F6]∞ Single Layers with Widely Divergent Second Harmonic Generation Effects211A Fluorooxosilicophosphate with an Unprecedented SiO2F4 Species56Assisting the Effective Design of Polar Iodates with Early Transition-Metal Oxide Fluoride Anions206Designing Deep‐UV Birefringent Crystals by Cation Regulation57Sn[B2O3F2]—The First Tin Fluorooxoborate as Possible NLO Material102Expanding Frontiers of Ultraviolet Nonlinear Optical Materials with Fluorophosphates265Fluorooxoborates: Ushering in a New Era of Deep Ultraviolet Nonlinear Optical Materials102Module-Guided Design Scheme for Deep-Ultraviolet Nonlinear Optical Materials195Removal of A-Site Alkali and Alkaline Earth Metal Cations in KBe2BO3F2-Type Layered Structures To Enhance the Deep-Ultraviolet Nonlinear Optical Capability46Centrosymmetric (NH4)2SbCl(SO4)2 and Non-centrosymmetric (NH4)SbCl2(SO4): Synergistic Effect of Hydrogen-Bonding Interactions and Lone-Pair Cations on the Framework Structures and Macroscopic Centricities89Ba 4 Bi 2 (Si 8−x B 4+x O 29 ) ( x = 0.09): a new acentric metal borosilicate as a promising nonlinear optical material53Pb 2 GaF 2 (SeO 3 ) 2 Cl: Band Engineering Strategy by Aliovalent Substitution for Enlarging Bandgap while Keeping Strong Second Harmonic Generation Response178Investigations of electronic and nonlinear optical properties of single alkali metal adsorbed graphene, graphyne and graphdiyne systems by first-principles calculations155BaB8O12F2: a promising deep-UV birefringent material60Ba3(C3N3O3)2: A New Phase of Barium Cyanurate Containing Parallel π-Conjugated Groups as a Birefringent Material Replacement for Calcite62A 2 SrM IV S 4 (A = Li, Na; M IV = Ge, Sn) concurrently exhibiting wide bandgaps and good nonlinear optical responses as new potential infrared nonlinear optical materials78A rich structural chemistry in π-conjugated hydroisocyanurates: layered structures of A 2 B(H 2 C 3 N 3 O 3 ) 4 · n H 2 O (A = K, Rb, Cs; B = Mg, Ca; n = 4, 10) with high ultraviolet transparency and strong optical anisotropy47Centrosymmetric K 2 SO 4 ·(SbF 3 ) 2 and noncentrosymmetric Rb 2 SO 4 ·(SbF 3 ) 2 resulting from cooperative effects of lone pair and cation size63LiO 4 tetrahedra lock the alignment of π-conjugated layers to maximize optical anisotropy in metal hydroisocyanurates44Targeting the Next Generation of Deep-Ultraviolet Nonlinear Optical Materials: Expanding from Borates to Borate Fluorides to Fluorooxoborates450CsSbF 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 Structure432Module-Analysis-Assisted Design of Deep Ultraviolet Fluorooxoborates with Extremely Large Gap and High Structural Stability109BaB 2 O 3 F 2 : A Barium Fluorooxoborate with a Unique [B 2 O 3 F] − Layer and Short Cutoff Edge38Prediction of Fluorooxoborates with Colossal Second Harmonic Generation (SHG) Coefficients and Extremely Wide Band Gaps: Towards Modulating Properties by Tuning the BO 3 /BO 3 F Ratio in Layers99Agar and egg shell derived calcium carbonate and calcium hydroxide nanoparticles: Synthesis, characterization and applications61Facile Growth of an Ultraviolet Hydroisocyanurate Crystal with Strong Nonlinearity and a Wide Phase-Matching Region from π-Conjugated (HC3N3O3)2– Groups45Nitrate nonlinear optical crystals: A survey on structure-performance relationships146Nontoxic KBBF Family Member Zn2BO3(OH): Balance between Beneficial Layered Structure and Layer Tendency81Sn2B5O9Cl: A Material with Large Birefringence Enhancement Activated Prepared via Alkaline‐Earth‐Metal Substitution by Tin255First-Principles Design and Simulations Promote the Development of Nonlinear Optical Crystals299A new family of quaternary thiosilicates SrA 2 SiS 4 (A = Li, Na, Cu) as promising infrared nonlinear optical crystals48Emergent Deep‐Ultraviolet Nonlinear Optical Candidates324Neue Kandidaten für die nichtlineare Optik im Tief‐UV‐Bereich43A review of the AI2B II C IV DVI4 family as infrared nonlinear optical materials: the effect of each site on the structure and optical properties59PbSrSiO 4 : a new ultraviolet nonlinear optical material with a strong second harmonic generation response and moderate birefringence37RbB 3 O 4 F 2 : a rubidium fluorooxoborate with an unprecedented [B 3 O 5 F 2 ] 3− functionalized unit and a large birefringence37Two-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 triangles146PbB5O7F3: A High-Performing Short-Wavelength Nonlinear Optical Material120Designing Silicates as Deep‐UV Nonlinear Optical (NLO) Materials using Edge‐Sharing Tetrahedra147Designing Silicates as Deep‐UV Nonlinear Optical (NLO) Materials using Edge‐Sharing Tetrahedra43Lead 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 Materials55Alignment of Polar Moieties Leading to Strong Second Harmonic Response in KCsMoP2O951ZnIO3F: Zinc Iodate Fluoride with Large Birefringence and Wide Band Gap57Enhanced nonlinear optical functionality in birefringence and refractive index dispersion of the deep-ultraviolet fluorooxoborates123Designing a Deep-UV Nonlinear Optical Fluorooxosilicophosphate127K4Sb(SO4)3Cl: The first apatite-type sulfate ultraviolet nonlinear optical material with sharply enlarged birefringence61A 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 principles45New Alkaline-Earth Metal Fluoroiodates Exhibiting Large Birefringence and Short Ultraviolet Cutoff Edge with Highly Polarizable (IO 3 F) 2– Units63Two Pyrophosphates with Large Birefringences and Second‐Harmonic Responses as Ultraviolet Nonlinear Optical Materials137Structure-property survey and computer-assisted screening of mid-infrared nonlinear optical chalcohalides113First-Principles High-Throughput Screening Pipeline for Nonlinear Optical Materials: Application to Borates106K 2 Sb(P 2 O 7 )F: Cairo Pentagonal Layer with Bifunctional Genes Reveal Optical Performance297K2Sb(P2O7)F: Cairo Pentagonal Layer with Bifunctional Genes Reveal Optical Performance38Realizing Deep-Ultraviolet Second Harmonic Generation by First-Principles-Guided Materials Exploration in Hydroxyborates111Pb 18 O 8 Cl 15 I 5 : A Polar Lead Mixed Oxyhalide with Unprecedented Architecture and Excellent Infrared Nonlinear Optical Properties165In Silico Modeling of New “Y-Series”-Based Near-Infrared Sensitive Non-Fullerene Acceptors for Efficient Organic Solar Cells134Recent Advances in Oxide‐based Nonlinear Optical Materials with Wide Infrared Transparency Beyond 6 μm38A 3 BBi(P 2 O 7 ) 2 (A = Rb, Cs; B = Pb, Ba): Isovalent Cation Substitution to Sustain Large Second-Harmonic Generation Responses106Series of Crystals with Giant Optical Anisotropy: A Targeted Strategic Research140α‐SnF 2 : A UV Birefringent Material with Large Birefringence and Easy Crystal Growth210NaZnCO 3 (OH): A High-Performance Carbonate Ultraviolet Nonlinear Optical Crystal Derived from KBe 2 BO 3 F 2194From silicates to oxonitridosilicates: improving optical anisotropy for phase-matching as ultraviolet nonlinear optical materials47Borates: A Rich Source for Optical Materials1089KNa2ZrF7: A Mixed-Metal Fluoride Exhibits Phase-Matchable Second-Harmonic-Generation Effect and High Laser-Induced Damage Threshold42Sn2B5O9Br as an Outstanding Bifunctional Material with Strong Second‐Harmonic Generation Effect and Large Birefringence84Computationally assisted multistage design and prediction driving the discovery of deep-ultraviolet nonlinear optical materials41Recent advances of oxyfluorides for nonlinear optical applications69To improve the key properties of nonlinear optical crystals assembled with tetrahedral functional building units46Prediction of Novel van der Waals Boron Oxides with Superior Deep‐Ultraviolet Nonlinear Optical Performance43K5Mg2La3(BO3)6: An Efficient, Deep-Ultraviolet Nonlinear Optical Material70Unique Unilateral-Chelated Mode-Induced d–p−π Interaction Enhances Second-Harmonic Generation Response in New Ln3LiMS7 Family41Fluorine‐Driven Enhancement of Birefringence in the Fluorooxosulfate: A Deep Evaluation from a Joint Experimental and Computational Study139BaYOBO3: A deep-ultraviolet rare-earth oxy-borate with a large second harmonic generation response45Exploring Deep-UV Nonlinear Optical Materials with Enhanced Second Harmonic Generation Response and Birefringence in Fluoroaluminoborate Crystals69Sn2PO4I: An Excellent Birefringent Material with Giant Optical Anisotropy in Non π‐Conjugated Phosphate2122D van der Waals Layered [C(NH2)3]2SO3S Exhibits Desirable UV Nonlinear-Optical Trade-Off47La 3 Ga 3 Ge 2 S 3 O 10 : An Ultraviolet Nonlinear Optical Oxysulfide Designed by Anion‐Directed Band Gap Engineering63Complex coordinated functional groups: A great genes for nonlinear optical materials64Na4B8O9F10: A Deep‐Ultraviolet Transparent Nonlinear Optical Fluorooxoborate with Unexpected Short Phase‐Matching Wavelength Induced by Optimized Chromatic Dispersion133Ball milling induced strong polarization electric fields in Cu3B2O6 crystals for high efficiency piezocatalysis90Achieving a strong second harmonic generation response and a wide band gap in a Hg-based material41Halogen regulation triggers structural transformation from centrosymmetric to noncentrosymmetric switches in tin phosphate halides Sn 2 PO 4 X (X = F, Cl)47Large optical anisotropy-oriented construction of a carbonate-nitrate chloride compound as a potential ultraviolet birefringent material44Rational design of a promising oxychalcogenide infrared nonlinear optical crystal60Sc 2 F 2 (B 2 O 5 ): a deep ultraviolet scandium borate fluoride exhibiting large birefringence induced by the synergistic effect of B 2 O 5 and ScO n F 2 groups38Unprecedented mid-infrared nonlinear optical materials achieved by crystal structure engineering, a case study of (KX)P 2 S 6 (X = Sb, Bi, Ba)59Potential optical functional crystals with large birefringence: Recent advances and future prospects322Sulfamide: A Promising Deep‐Ultraviolet Nonlinear Optical Crystal Assembled from Polar Covalent [SO2(NH2)2] Tetrahedra84The Combination of Structure Prediction and Experiment for the Exploration of Alkali‐Earth Metal‐Contained Chalcopyrite‐Like IR Nonlinear Optical Material104Noncentrosymmetric Rare-Earth Borate Fluoride La2B5O9F3: A New Ultraviolet Nonlinear Optical Crystal with Enhanced Linear and Nonlinear Performance48Lone Pair-Driven Enhancement of Birefringence in Polar Alkali Metal Antimony Phosphates46Promising Deep‐Ultraviolet Birefringent Materials via Rational Design and Assembly of Planar π‐Conjugated [B(OH)3] and [B3O3(OH)3] Functional Species83Double‐Modification Oriented Design of a Deep‐UV Birefringent Crystal Functionalized by [B12O16F4(OH)4] Clusters139(NH4)3B11PO19F3: a deep-UV nonlinear optical crystal with unique [B5PO10F]∞ layers142Two Metal Phosphate Nonlinear Optical Materials Simultaneously Exhibiting Ultraviolet Transparence and a Large Birefringence50[Ba2F2][Ge2O3S2]: An Unprecedented Heteroanionic Infrared Nonlinear Optical Material Containing Three Typical Anions47An excellent deep-ultraviolet birefringent material based on [BO2]∞ infinite chains185Deep Ultraviolet-Transparent Materials with Strong Second-Harmonic Response50Design of novel deep-UV nonlinear optical materials with one-dimensional functional module [BO2]∞ chain and fluorine-driven short phase-matching43Exploring Short-Wavelength Phase-Matching Nonlinear Optical Crystals by Employing KBe2BO3F2 as the Template95K 3 C 6 N 7 O 3 ·2H 2 O: A Multifunctional Nonlinear Optical Cyamelurate Crystal with Colossal π-Conjugated Orbitals44AIB3IIC3IIIQ8VI: A New Family for the Design of Infrared Nonlinear Optical Materials by Coupling Octahedra and Tetrahedra Units152Rb 2 CdSi 4 S 10 : novel [Si 4 S 10 ] T2-supertetrahedra-contained infrared nonlinear optical material with large band gap79Rb 3 B 11 P 2 O 23 : Materials Design of a New Chemically Benign Deep-Ultraviolet Nonlinear Optical Material58Aluminoborates as Nonlinear Optical Materials79Accurate design and synthesis of nonlinear optical crystals employing KBe2BO3F2 as structural template55Anisotropic structure building unit involving diverse chemical bonds: a new opportunity for high-performance second-order NLO materials181Evaluating refractive index and birefringence of nonlinear optical crystals: Classical methods and new developments45Unbiased Screening of Novel Infrared Nonlinear Optical Materials with High Thermal Conductivity: Long‐neglected Nitrides and Popular Chalcogenides48NaRb 6 (B 4 O 5 (OH) 4 ) 3 (BO 2 ) Featuring Noncentrosymmetry, Chirality, and the Linear Anionic Group BO 2 –100Clamping effect driven design and fabrication of new infrared birefringent materials with large optical anisotropy45Recent Development of Sn II , Sb III ‐based Birefringent Material: Crystal Chemistry and Investigation of Birefringence130Target‐Driven Design of Deep‐UV Nonlinear Optical Materials via Interpretable Machine Learning125Chain‐like [S x ] ( x =2–6) Units Realizing Giant Birefringence with Transparency in the Near‐Infrared for Optoelectronic Materials53Na3SiS3F: A Wide Bandgap Fluorothiosilicate with Unique [SiS3F] Unit and High Laser‐Induced Damage Threshold39Cs 3 [(BOP) 2 (B 3 O 7 ) 3 ]: A Deep-Ultraviolet Nonlinear Optical Crystal Designed by Optimizing Matching of Cation and Anion Groups169Improved Birefringence Activated by Tetrahedra Decorated with a Single Linear Unit38From Monofluorophosphates A2PO3F to Difluorophosphates APO2F2 (A = alkali metal): Design of a Potential Deep-Ultraviolet Nonlinear Optical Materials System with a Shortened Phase-Matching Wavelength41Zn 2 HgP 2 S 8 : A Wide Bandgap Hg‐Based Infrared Nonlinear Optical Material with Large Second‐Harmonic Generation Response75A prediction-driven database to enable rapid discovery of nonlinear optical materials46Deep‐Ultraviolet Transparent Mixed Metal Sulfamates with Enhanced Nonlinear Optical Properties and Birefringence75Fluorination Strategy Towards Symmetry Breaking of Boron‐centered Tetrahedron for Poly‐fluorinated Optical Crystals70Fluorination strategy toward chemical and functional modification65Recent advances in rational structure design for nonlinear optical crystals: leveraging advantageous templates153Cs 3 In(In 4 Se 7 )(P 2 Se 6 ): A Multi‐Chromophore Chalcogenide with Excellent Nonlinear Optical Property Designed by Group Grafting55Toward the ultraviolet (UV) or deep-UV nonlinear optical crystals: The combination of π-conjugated planar [XY3] and tetrahedral [XY4]80Record Second-Harmonic Generation and Birefringence in an Ultraviolet Antimonate by Bond Engineering157Rational Combination of π‐Conjugated and Non‐π‐Conjugated Groups Achieving Strong Nonlinear Optical Response, Large Optical Anisotropy, and UV Light‐Switchable Fluorescence65Review on birefringence in borates based on birefringence-active functional groups and arrangements57Functional Modules Map of Unexplored Chemical Space: Guiding the Discovery of Giant Birefringent Materials76Exploiting Deep‐Ultraviolet Nonlinear Optical Material Rb 2 ScB 3 O 6 F 2 Originated from Congruously Oriented [B 3 O 6 ] Groups61Computer‐Aided Development of New Nonlinear Optical Materials38Looking Back the Nonlinear Optical Crystals in a Functionalized Unit's Perspective109Chalcophosphates: A plentiful source of infrared nonlinear optical materials42A Promising Deep Ultraviolet Nonlinear Optical Crystal Activated by the Ordered Structure Design40

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  4. Cs 3 VO(O 2 ) 2 CO 3 : an exceptionally thermostable carbonatoperoxovanadate with an extremely large second-harmonic generation response

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  34. Expanding Frontiers of Ultraviolet Nonlinear Optical Materials with Fluorophosphates

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  38. Removal of A-Site Alkali and Alkaline Earth Metal Cations in KBe2BO3F2-Type Layered Structures To Enhance the Deep-Ultraviolet Nonlinear Optical Capability

    Inorganic Chemistry · 2018-08-15

    Lei Kang, Zheshuai Lin, Feng Liu, Bing Qiang Huang

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  39. Two new mixed metal borates with the large birefringence in borates system confirmed by a disordered crystal optical calculation method

    Journal of Alloys and Compounds · 2018-09-01

    Xueyan Zhang, Shichao Cheng, Ming Wen, Hongyi Li, Jun Zhang

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  40. Synthesis, crystal structures and nonlinear optical properties of polymorphism: α- and β-RbHgI3·H2O

    Journal of Alloys and Compounds · 2018-09-04

    Ling Huang, Qian Wang, Fangfang He, Xiaoyan Liu, Ziwei Chen, Wen Jun He, Xueying Luo, Daojiang Gao, Jian Bi, Guohong Zou

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  41. Centrosymmetric (NH4)2SbCl(SO4)2 and Non-centrosymmetric (NH4)SbCl2(SO4): Synergistic Effect of Hydrogen-Bonding Interactions and Lone-Pair Cations on the Framework Structures and Macroscopic Centricities

    Crystal Growth & Design · 2018-09-11

    Fangfang He, Qian Wang, Cuifang Hu, Wen Jun He, Xueying Luo, Ling Huang, Daojiang Gao, Jian Bi, Xin Wang, Guohong Zou

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  42. NaCa4V5O17 with isolated V2O7 dimer and V3O10 trimer exhibiting a large birefringence

    Journal of Solid State Chemistry · 2018-09-12

    Zhiqing Xie, Shichao Cheng, Shuwei Li, Hanqin Ding

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  43. Synthesis, Structure, and Properties of the Non-Centrosymmeteric Compound LiNaRbB5O8(OH)2

    Crystal Growth & Design · 2018-09-21

    Yi Jin Yang, Yi Qiu, Pifu Gong, Qian Huang, Sangen Zhao, Siyang Luo, Junliang Sun, Zheshuai Lin

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  44. Structure–Property Relationship and Systematic Study of a Series of Terpyridine Based Nonlinear Optical Compounds: DFT Computation of Interactive Design

    Journal of Cluster Science · 2018-09-28

    Muhammad Ramzan Saeed Ashraf Janjua

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  45. Na4Yb(CO3)3F: A New UV Nonlinear Optical Material with a Large Second Harmonic Generation Response

    Crystals · 2018-09-30

    Qiaoling Chen, Min Luo, Chensheng Lin

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  46. Na 3 B 7 O 11 F 2 : a new sodium-rich fluorooxoborate with a unique [B 14 O 24 F 4 ] ring and a short ultraviolet absorption edge

    Dalton Transactions · 2018-10-18

    Changcheng Tang, Xingxing Jiang, Wenlong Yin, Lijuan Liu, Mingjun Xia, Qian Huang, Gaomin Song, Xiaoyang Wang, Zheshuai Lin, Chuangtian Chen

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  47. The linear and nonlinear optical response of CsGeX3 (X=Cl, Br, and I): The finite field and first-principles investigation

    Optik · 2018-10-25

    Qiaoqiao Zhang, Hahaer Mushahali, Haiming Duan, Ming‐Hsien Lee, Qun Jing

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  48. Ba 4 Bi 2 (Si 8−x B 4+x O 29 ) ( x = 0.09): a new acentric metal borosilicate as a promising nonlinear optical material

    Chemical Science · 2018-10-31

    Ru‐Ling Tang, Chun‐Li Hu, Fei‐Fei Mao, Jiang-He Feng, Jiang‐Gao Mao

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  49. Size effect and identified superior functional units enhancing second harmonic generation responses on the II-IV-V2 type nonlinear optical crystals

    Chemical Physics · 2018-11-13

    Guijie He, Ilmira Rozahun, Zhi Li, Jun Zhang, Ming‐Hsien Lee

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

    Inorganic Chemistry · 2018-11-14

    Fengjiao Guo, Jian Wei Han, Jianian Cheng, Zhihua Yang, Miriding Mutailipu, Shilie Pan

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