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RESEARCH PAPER · Journal of the American Chemical Society · 2017

Finding the Next Deep-Ultraviolet Nonlinear Optical Material: NH4B4O6F

Guoqiang Q. Shi, Ying Wang, Fangfang Zhang, Bingbing Zhang, Zhihua Yang, Xueling Hou, Shilie Pan, Kenneth Reinhard Poeppelmeier

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Finding the Next Deep-Ultraviolet Nonlinear Optical Material: NH4B4O6FOriginalRational Design of Deep-Ultraviolet Nonlinear Optical Materials in Fluorooxoborates: Toward Optimal Planar Configuration158CsB 4 O 6 F: A Congruent‐Melting Deep‐Ultraviolet Nonlinear Optical Material by Combining Superior Functional Units185CsB4O6F: A Congruent‐Melting Deep‐Ultraviolet Nonlinear Optical Material by Combining Superior Functional Units895New Compressed Chalcopyrite-like Li2BaMIVQ4 (MIV = Ge, Sn; Q = S, Se): Promising Infrared Nonlinear Optical Materials246Viewpoint: Inorganic Materials for UV and Deep-UV Nonlinear-Optical Applications207The Next‐Generation of Nonlinear Optical Materials: Rb3Ba3Li2Al4B6O20F—Synthesis, Characterization, and Crystal Growth87The First Alkaline‐Earth Fluorooxoborate Ba[B4O6F2]—Characterisation and Doping with Eu2+95Chemical Cosubstitution-Oriented Design of Rare-Earth Borates as Potential Ultraviolet Nonlinear Optical Materials268Cs 3 VO(O 2 ) 2 CO 3 : an exceptionally thermostable carbonatoperoxovanadate with an extremely large second-harmonic generation response129Li 8 NaRb 3 (SO 4 ) 6 ·2H 2 O as a new sulfate deep-ultraviolet nonlinear optical material93Oxyhalides: prospecting ore for optical functional materials with large laser damage thresholds76Perfect balance harmony in Ba 2 NO 3 (OH) 3 : a beryllium-free nitrate as a UV nonlinear optical material184The first lead fluorooxoborate PbB 5 O 8 F: achieving the coexistence of large birefringence and deep-ultraviolet cut-off edge76Cation‐Tuned Synthesis of Fluorooxoborates: Towards Optimal Deep‐Ultraviolet Nonlinear Optical Materials192Cation‐Tuned Synthesis of Fluorooxoborates: Towards Optimal Deep‐Ultraviolet Nonlinear Optical Materials714From AgGaS2 to Li2ZnSiS4: Realizing Impressive High Laser Damage Threshold Together with Large Second-Harmonic Generation Response134Functional Materials Design via Structural Regulation Originated from Ions Introduction: A Study Case in Cesium Iodate System91Non-Centrosymmetric RbNaMgP 2 O 7 with Unprecedented Thermo-Induced Enhancement of Second Harmonic Generation240Pushing Nonlinear Optical Oxides into the Mid-Infrared Spectral Region Beyond 10 μm: Design, Synthesis, and Characterization of La3SnGa5O14147SrB 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 Materials116Pb2BO3I: A Borate Iodide with the Largest Second‐Harmonic Generation (SHG) Response in the KBe2BO3F2 (KBBF) Family of Nonlinear Optical (NLO) Materials238A 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 Materials357The role of cations in second-order nonlinear optical materials based on π-conjugated [BO 3 ] 3− groups193CaB5O7F3: A Beryllium-Free Alkaline-Earth Fluorooxoborate Exhibiting Excellent Nonlinear Optical Performances192Polar Fluorooxoborate, NaB4O6F: A Promising Material for Ionic Conduction and Nonlinear Optics495NH4Be2BO3F2 and γ‐Be2BO3F: Overcoming the Layering Habit in KBe2BO3F2 for the Next‐Generation Deep‐Ultraviolet Nonlinear Optical Materials282Rational Design of the First Lead/Tin Fluorooxoborates MB2O3F2 (M = Pb, Sn), Containing Flexible Two-Dimensional [B6O12F6]∞ Single Layers with Widely Divergent Second Harmonic Generation Effects212Assisting the Effective Design of Polar Iodates with Early Transition-Metal Oxide Fluoride Anions207Sn[B2O3F2]—The First Tin Fluorooxoborate as Possible NLO Material102Advantageous Units in Antimony Sulfides: Exploration and Design of Infrared Nonlinear Optical Materials95Expanding Frontiers of Ultraviolet Nonlinear Optical Materials with Fluorophosphates266Fluorooxoborates: Ushering in a New Era of Deep Ultraviolet Nonlinear Optical Materials102Module-Guided Design Scheme for Deep-Ultraviolet Nonlinear Optical Materials197Ba3Mg3(BO3)3F3 polymorphs with reversible phase transition and high performances as ultraviolet nonlinear optical materials471Effects of transition metals on physical properties of M2BC (M = V, Nb, Mo and Ta): A DFT calculation80Rational Design of a LiNbO3-like Nonlinear Optical Crystal, Li2ZrTeO6, with High Laser-Damage Threshold and Wide Mid-IR Transparency Window152BaB2S4: An Efficient and Air-Stable Thioborate as Infrared Nonlinear Optical Material with High Laser Damage Threshold86Designing an Excellent Deep-Ultraviolet Birefringent Material for Light Polarization537Pb 2 GaF 2 (SeO 3 ) 2 Cl: Band Engineering Strategy by Aliovalent Substitution for Enlarging Bandgap while Keeping Strong Second Harmonic Generation Response178A 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 materials78Co-crystal LiCl·(H 3 C 3 N 3 O 3 ): a promising solar-blind nonlinear optical crystal with giant nonlinearity from coplanar π-conjugated groups78K 2 SrP 4 O 12 : a deep-UV transparent cyclophosphate as a nonlinear optical crystal79Rational Design via Synergistic Combination Leads to an Outstanding Deep-Ultraviolet Birefringent Li2Na2B2O5 Material with an Unvalued B2O5 Functional Gene284Lone‐Pair Enhanced Birefringence in an Alkaline‐Earth Metal Tin(II) Phosphate BaSn 2 (PO 4 ) 2131KLi(HC 3 N 3 O 3 )·2H 2 O: Solvent-drop Grinding Method toward the Hydro-isocyanurate Nonlinear Optical Crystal314Targeting the Next Generation of Deep-Ultraviolet Nonlinear Optical Materials: Expanding from Borates to Borate Fluorides to Fluorooxoborates453Module-Analysis-Assisted Design of Deep Ultraviolet Fluorooxoborates with Extremely Large Gap and High Structural Stability109Sr 6 Cd 2 Sb 6 O 7 S 10 : Strong SHG Response Activated by Highly Polarizable Sb/O/S Groups124Sr2LiScB4O10:Ce3+/Tb3+: A Green-Emitting Phosphor with High Energy Transfer Efficiency and Stability for LEDs and FEDs108Prediction 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 Layers99AHgSnQ4 (A = Sr, Ba; Q = S, Se): A Series of Hg-Based Infrared Nonlinear-Optical Materials with Strong Second-Harmonic-Generation Response and Good Phase Matchability76Nitrate nonlinear optical crystals: A survey on structure-performance relationships146Sn2B5O9Cl: A Material with Large Birefringence Enhancement Activated Prepared via Alkaline‐Earth‐Metal Substitution by Tin255Synthesis of Co3O4 Nano Aggregates by Co-precipitation Method and its Catalytic and Fuel Additive Applications81Li[LiCs2Cl][Ga3S6]: A Nanoporous Framework of GaS4 Tetrahedra with Excellent Nonlinear Optical Performance172First-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 484CsAlB 3 O 6 F: a beryllium-free deep-ultraviolet nonlinear optical material with enhanced thermal stability153(NH4)Bi2(IO3)2F5: An Unusual Ammonium‐Containing Metal Iodate Fluoride Showing Strong Second Harmonic Generation Response and Thermochromic Behavior92Emergent Deep‐Ultraviolet Nonlinear Optical Candidates327Inorganic planar π-conjugated groups in nonlinear optical crystals: review and outlook145PbB5O7F3: A High-Performing Short-Wavelength Nonlinear Optical Material121BaF 2 TeF 2 (OH) 2 : A UV Nonlinear Optical Fluorotellurite Material Designed by Band-Gap Engineering157Designing Silicates as Deep‐UV Nonlinear Optical (NLO) Materials using Edge‐Sharing Tetrahedra148Lead Mixed Oxyhalides Satisfying All Fundamental Requirements for High‐Performance Mid‐Infrared Nonlinear Optical Materials164Enhanced nonlinear optical functionality in birefringence and refractive index dispersion of the deep-ultraviolet fluorooxoborates123Theoretical and Conceptual Framework to Design Efficient Dye-Sensitized Solar Cells (DSSCs): Molecular Engineering by DFT Method153A review on phase transition and structure-performance relationship of second-order nonlinear optical polymorphs107Rational Design of the Metal‐Free KBe 2 BO 3 F 2 ⋅(KBBF) Family Member C(NH 2 ) 3 SO 3 F with Ultraviolet Optical Nonlinearity201Two 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 Performance297Realizing Deep-Ultraviolet Second Harmonic Generation by First-Principles-Guided Materials Exploration in Hydroxyborates112The study of structure evolvement of KTiOPO4 family and their nonlinear optical properties98Salt-Inclusion Chalcogenide [Ba4Cl2][ZnGa4S10]: Rational Design of an IR Nonlinear Optical Material with Superior Comprehensive Performance Derived from AgGaS2133Pb 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 Cells135Finding Optimal Mid-Infrared Nonlinear Optical Materials in Germanates by First-Principles High-Throughput Screening and Experimental Verification80A 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 Research139α‐SnF 2 : A UV Birefringent Material with Large Birefringence and Easy Crystal Growth209NaZnCO 3 (OH): A High-Performance Carbonate Ultraviolet Nonlinear Optical Crystal Derived from KBe 2 BO 3 F 2194Borates: A Rich Source for Optical Materials1097Sn2B5O9Br as an Outstanding Bifunctional Material with Strong Second‐Harmonic Generation Effect and Large Birefringence84A comprehensive survey on nonlinear optical phosphates: Role of multicoordinate groups106M(NH 2 SO 3 ) 2 (M=Sr, Ba): Two Deep‐Ultraviolet Transparent Sulfamates Exhibiting Strong Second Harmonic Generation Responses and Moderate Birefringence141Theoretical Framework for Encapsulation of Inorganic B12N12 Nanoclusters with Alkaline Earth Metals for Efficient Hydrogen Adsorption: A Step Forward toward Hydrogen Storage Materials81[C(NH2)3]3PO4·2H2O: A new metal-free ultraviolet nonlinear optical phosphate with large birefringence and second-harmonic generation response71Discovery of NLO Semiorganic (C 5 H 6 ON) + (H 2 PO 4 ) − : Dipole Moment Modulation and Superior Synergy in Solar-Blind UV Region270A Deep‐UV Nonlinear Optical Borosulfate with Incommensurate Modulations71Quantum chemical design of near‐infrared sensitive fused ring electron acceptors containing selenophene as π‐bridge for high‐performance organic solar cells79Toward the Enhancement of Critical Performance for Deep-Ultraviolet Frequency-Doubling Crystals Utilizing Covalent Tetrahedra137LiZn(OH)CO3: A Deep‐Ultraviolet Nonlinear Optical Hydroxycarbonate Designed from a Diamond‐like Structure179UV Solar‐Blind‐Region Phase‐Matchable Optical Nonlinearity and Anisotropy in a π‐Conjugated Cation‐Containing Phosphate194Discovery of First Magnesium Fluorooxoborate with Stable Fluorine Terminated Framework for Deep‐UV Nonlinear Optical Application168Expanding the chemistry of borates with functional [BO2]− anions200Fluorine‐Driven Enhancement of Birefringence in the Fluorooxosulfate: A Deep Evaluation from a Joint Experimental and Computational Study139Hydroxyfluorooxoborate Na[B3O3F2(OH)2]⋅[B(OH)3]: Optimizing the Optical Anisotropy with Heteroanionic Units for Deep Ultraviolet Birefringent Crystals147Li 4 MgGe 2 S 7 : The First Alkali and Alkaline‐Earth Diamond‐Like Infrared Nonlinear Optical Material with Exceptional Large Band Gap214Sn2PO4I: An Excellent Birefringent Material with Giant Optical Anisotropy in Non π‐Conjugated Phosphate212A General Principle for DUV NLO Materials: π‐Conjugated Confinement Enlarges Band Gap**175Achieving Short‐Wavelength Phase‐Matching Second Harmonic Generation in Boron‐Rich Borosulfate with Planar [BO3] Units102Strong SHG Responses in a Beryllium‐Free Deep‐UV‐Transparent Hydroxyborate via Covalent Bond Modification88Dimensionality reduction made high-performance mid-infrared nonlinear halide crystal74A Lanthanum Ammonium Sulfate Double Salt with a Strong SHG Response and Wide Deep‐UV Transparency96Na4B8O9F10: A Deep‐Ultraviolet Transparent Nonlinear Optical Fluorooxoborate with Unexpected Short Phase‐Matching Wavelength Induced by Optimized Chromatic Dispersion133Guanidinium Fluorooxoborates as Efficient Metal-free Short-Wavelength Nonlinear Optical Crystals140[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 units85Metal oxyhalides: an emerging family of nonlinear optical materials125Potential optical functional crystals with large birefringence: Recent advances and future prospects323Sulfamide: A Promising Deep‐Ultraviolet Nonlinear Optical Crystal Assembled from Polar Covalent [SO2(NH2)2] Tetrahedra84Toward the Rational Design of Mid‐Infrared Nonlinear Optical Materials with Targeted Properties via a Multi‐Level Data‐Driven Approach110Strong Nonlinearity Induced by Coaxial Alignment of Polar Chain and Dense [BO3] Units in CaZn2(BO3)2215Sr3[SnOSe3][CO3]: A Heteroanionic Nonlinear Optical Material Containing Planar π‐conjugated [CO3] and Heteroleptic [SnOSe3] Anionic Groups78The Combination of Structure Prediction and Experiment for the Exploration of Alkali‐Earth Metal‐Contained Chalcopyrite‐Like IR Nonlinear Optical Material105Promising Deep‐Ultraviolet Birefringent Materials via Rational Design and Assembly of Planar π‐Conjugated [B(OH)3] and [B3O3(OH)3] Functional Species82Double‐Modification Oriented Design of a Deep‐UV Birefringent Crystal Functionalized by [B12O16F4(OH)4] Clusters138Enhancement of Birefringence in Borophosphate Pushing Phase-Matching into the Short-Wavelength Region150All-small-molecule organic solar cells with high fill factor and enhanced open-circuit voltage with 18.25 % PCE: Physical insights from quantum chemical calculations79(NH4)3B11PO19F3: a deep-UV nonlinear optical crystal with unique [B5PO10F]∞ layers142Deep-ultraviolet nonlinear optical crystals: concept development and materials discovery181An excellent deep-ultraviolet birefringent material based on [BO2]∞ infinite chains186Exploring Short-Wavelength Phase-Matching Nonlinear Optical Crystals by Employing KBe2BO3F2 as the Template95AIB3IIC3IIIQ8VI: A New Family for the Design of Infrared Nonlinear Optical Materials by Coupling Octahedra and Tetrahedra Units151Rb 2 CdSi 4 S 10 : novel [Si 4 S 10 ] T2-supertetrahedra-contained infrared nonlinear optical material with large band gap79Aluminoborates as Nonlinear Optical Materials77Anisotropic structure building unit involving diverse chemical bonds: a new opportunity for high-performance second-order NLO materials180NaRb 6 (B 4 O 5 (OH) 4 ) 3 (BO 2 ) Featuring Noncentrosymmetry, Chirality, and the Linear Anionic Group BO 2 –101An interlinked prediction-experiment paradigm discovering deep-ultraviolet fluorooxoborates with desired optical nonlinearity and birefringence76Recent Development of Sn II , Sb III ‐based Birefringent Material: Crystal Chemistry and Investigation of Birefringence129Target‐Driven Design of Deep‐UV Nonlinear Optical Materials via Interpretable Machine Learning125Unveiling the Superior Optical Properties of Novel Melamine‐Based Nonlinear Optical Material with Strong Second‐Harmonic Generation and Giant Optical Anisotropy74Design of the Ionic Organic Nonlinear Optical Material NH 4 [LiC 3 H(CH 3 )O 4 ] with Ultrawide Band Gap and Moderate Birefringence79Cs 3 [(BOP) 2 (B 3 O 7 ) 3 ]: A Deep-Ultraviolet Nonlinear Optical Crystal Designed by Optimizing Matching of Cation and Anion Groups169Zn 2 HgP 2 S 8 : A Wide Bandgap Hg‐Based Infrared Nonlinear Optical Material with Large Second‐Harmonic Generation Response75Breaking the Inherent Interarrangement of [B3O6] Clusters for Nonlinear Optics with Orbital Hybridization Enhancement143Highly Birefringent d 0 Transition Metal Fluoroantimonite in the Mid Infrared Band: Order–Disorder Regulation by Cationic Size84Deep‐Ultraviolet Transparent Mixed Metal Sulfamates with Enhanced Nonlinear Optical Properties and Birefringence75“Three‐in‐One”: A New Hg‐Based Selenide Hg 7 P 2 Se 12 Exhibiting Wide Infrared Transparency Range and Strong Nonlinear Optical Effect80Recent advances in rational structure design for nonlinear optical crystals: leveraging advantageous templates153Record Second-Harmonic Generation and Birefringence in an Ultraviolet Antimonate by Bond Engineering157Assembly of π‐Conjugated [B3O6] Units by Mer‐Isomer [YO3F3] Octahedra to Design a UV Nonlinear Optical Material, Cs2YB3O6F296Enhanced UV Nonlinear Optical Properties in Layered Germanous Phosphites through Functional Group Sequential Construction116Functional Modules Map of Unexplored Chemical Space: Guiding the Discovery of Giant Birefringent Materials77Looking Back the Nonlinear Optical Crystals in a Functionalized Unit's Perspective109Decoupling the SHG‐Birefringence Trade‐off in UV NLO Materials via Triple‐Control Coordination Engineering: Achieving Synergistic Performance Optimization88Vacuum ultraviolet second-harmonic generation in NH4B4O6F crystal73

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    Journal of Materials Chemistry C · 2018-01-01

    Zhihua Yang, Cong Hu, Miriding Mutailipu, Yanzhou Sun, Kui Wu, Min Zhang, Shilie Pan

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  38. Pb 3 (SeO 3 )Br 4 : a new nonlinear optical material with enhanced SHG response designed via an ion-substitution strategy

    Dalton Transactions · 2018-01-01

    Xiaoxiao Wang, Xingxing Jiang, Hongming Liu, Lei Yang, Zheshuai Lin, Zhanggui Hu, Xiang‐Gao Meng, Xingguo Chen, Jingui Qin

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  39. PbFePO 4 F 2 with a 1/6th bond depleted triangular lattice

    Dalton Transactions · 2018-01-01

    Hongcheng Lu, Hiroshi Kageyama

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  40. Perfect balance harmony in Ba 2 NO 3 (OH) 3 : a beryllium-free nitrate as a UV nonlinear optical material

    Chemical Communications · 2018-01-01

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  41. RbSe 3 B 2 O 9 (OH) and CsSe 3 B 2 O 9 (OH): one dimensional boroselenite-based anionic frameworks with second harmonic generation properties

    Dalton Transactions · 2018-01-01

    Jian‐Han Zhang, Qibing Wang, Chun-Le Chen, Ju-Xiang Luo, Chun‐Li Hu, Jun‐Ling Song, Jiang‐Gao Mao

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  42. Structural insights into T 2 -cluster-containing chalcogenides with vertex-, edge- and face-sharing connection modes of NaQ 6 ligands: Na 3 ZnM III Q 4 (M III = In, Ga; Q = S, Se)

    Dalton Transactions · 2018-01-01

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  43. Synthesis, crystal structure and optical properties of a new fluorocarbonate with an interesting sandwich-like structure

    Dalton Transactions · 2018-01-01

    Changcheng Tang, Xingxing Jiang, Shu Hai Guo, Mingjun Xia, Lijuan Liu, Xiaoyang Wang, Zheshuai Lin, Chuangtian Chen

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  44. The first lead fluorooxoborate PbB 5 O 8 F: achieving the coexistence of large birefringence and deep-ultraviolet cut-off edge

    Chemical Communications · 2018-01-01

    Miriding Mutailipu, Min Zhang, Bingbing Zhang, Zhihua Yang, Shilie Pan

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  45. A Member of Fluorooxoborates: Li2Na0.9K0.1B5O8F2 with the Fundamental Building Block B5O10F2 and a Short Cutoff Edge

    Inorganic Chemistry · 2018-01-02

    Shujuan Han, Ying Wang, Bingbing Zhang, Zhihua Yang, Shilie Pan

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

    Angewandte Chemie · 2018-01-10

    Ying Wang, Bingbing Zhang, Zhihua Yang, Shilie Pan

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

    Angewandte Chemie International Edition · 2018-01-10

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  48. A Joint Strategy To Evaluate the Microscopic Origin of the Second-Harmonic-Generation Response in Nonpolar ABCO3F Compounds

    Inorganic Chemistry · 2018-01-17

    Qun Jing, Guang Yang, Zhaohui Chen, Xiaoyu Dong, Yunjing Shi

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  49. From AgGaS2 to Li2ZnSiS4: Realizing Impressive High Laser Damage Threshold Together with Large Second-Harmonic Generation Response

    Chemistry of Materials · 2018-01-17

    Guangmao Li, Yu Chu, Zhongxiang Zhou

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  50. Functional Materials Design via Structural Regulation Originated from Ions Introduction: A Study Case in Cesium Iodate System

    Chemistry of Materials · 2018-01-18

    Min Zhang, Cong Hu, Tushagu Abudouwufu, Zhihua Yang, Shilie Pan

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