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RESEARCH PAPER · Nature Photonics · 2023

Achieving the full-wavelength phase-matching for efficient nonlinear optical frequency conversion in C(NH2)3BF4

Miriding Mutailipu, Jian Wei Han, Zhi Li, Fuming Li, Junjie Li, Fangfang Zhang, Xifa Long, Zhihua Yang, Shilie Pan

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Achieving the full-wavelength phase-matching for efficient nonlinear optical frequency conversion in C(NH2)3BF4OriginalA new infrared nonlinear optical material BaZnGeS 4 with a wide band gap and large nonlinear optical response34From CdPb 8 (SeO 3 ) 4 Br 10 to Pb 3 (TeO 3 )Br 4 : the first tellurite bromide exhibiting an SHG response and mid-IR transparency21Heteroanion-introduction-driven birefringence enhancement in oxychalcogenide Ba 3 M II Ge 3 O 2 S 8 (M II = Mn, Cd)19Hydroxyfluorooxoborate (NH 4 )[C(NH 2 ) 3 ][B 3 O 3 F 4 (OH)] for exploring the effects of cation substitution on structure and optical properties26K 5 [B 3 O 3 F 4 (OH)] 2 (NO 3 ): the first hydroxyfluorooxoborate-nitrate with a short ultraviolet cutoff edge and large birefringence18Ultraviolet Crystal with Strong Optical Nonlinearity by Creating Halogen-Centered Secondary Building Blocks15The unexpected salamo-type copper(II) complex: Synthesis, structure, theoretical calculations and fluorescence properties33Zn 2 HgP 2 S 8 : A Wide Bandgap Hg‐Based Infrared Nonlinear Optical Material with Large Second‐Harmonic Generation Response75Quadruple‐Bidentate Nitrate‐Ligated A 2 Hg(NO 3 ) 4 (A=K, Rb): Strong Second‐Harmonic Generation and Sufficient Birefringence59A survey of stereoactive oxysalts for linear and nonlinear optical applications40Rational Design of Noncentrosymmetric Organic–Inorganic Hybrids with a π-Conjugated Pyridium-Type Cation for High Nonlinear-Optical Performance19Enhanced ammonia gas sensing by cost-effective SnO2 gas sensor: Influence of effective Mo doping40Four UV Transparent Linear and Nonlinear Optical Materials Explored from Pure Selenite Compounds22LiGa(IO3)4: An Excellent NLO Material with Unprecedented 2D [Ga(IO3)4]∞− Layer Synthesized by Aliovalent Substitution20Mixed Anionic Tetrahedra Guided Design of New Infrared Nonlinear Optical Material Cs 3 Ga 8 S 13 Cl with High Laser‐Induced Damage Threshold26Excellent Nonlinear Optical M[M4Cl][Ga11S20] (M = A/Ba, A = K, Rb) Achieved by Unusual Cationic Substitution Strategy20Sr(NO 3 )(NH 2 SO 3 )·H 2 O: First Nitrate Sulfamate Revealing Remarkable Second Harmonic Generation and Optimized Birefringence25Double alkaline earth metals sulfide SrMgGeS4 with high laser-induced damage threshold and strong second-harmonic generation29Theoretical investigations on ternary defective diamond-like infrared nonlinear optical materials in Be-Ga-Se system18(SO3CF3)−: A Non‐π‐Conjugated Motif for Nonlinear Optical Crystals Transparent into the Deep‐Ultraviolet Region23A prediction-driven database to enable rapid discovery of nonlinear optical materials46Ln 2 F 2 (OH 2 )(MoO 3 ) 2 (SeO 3 ) 2 : Promising Multifunctional Nonlinear Optical Materials Created by Partial Fluorination Strategy under Corrosion Resistant Supercritical Reactions25Breaking the Inherent Interarrangement of [B3O6] Clusters for Nonlinear Optics with Orbital Hybridization Enhancement142Highly Birefringent d 0 Transition Metal Fluoroantimonite in the Mid Infrared Band: Order–Disorder Regulation by Cationic Size83Two UV organic-inorganic hybrid antimony-based materials with superior optical performance derived from cation-anion synergetic interactions30Designing Sulfate Crystals with Strong Optical Anisotropy through π‐Conjugated Tailoring51New Functional Groups Design toward High Performance Ultraviolet Nonlinear Optical Materials95Theoretical study of static and frequency-dependent nonlinear optical properties of 1-phenyl-2,5-di(thiophen-2-yl)-1H-pyrrole based D-π-A chromophores through π-linkers modifications: A gateway towards giant nonlinear optical compounds16A I B 3 II C 2 III Q 6 VI X VII : A Thioborate Halide Family for Developing Wide Bandgap Infrared Nonlinear Materials by Coupling Planar [BS 3 ] and Polycations25Fluorination Strategy Towards Symmetry Breaking of Boron‐centered Tetrahedron for Poly‐fluorinated Optical Crystals15Fluorination Strategy Towards Symmetry Breaking of Boron‐centered Tetrahedron for Poly‐fluorinated Optical Crystals70Mg(C3O4H2)(H2O)2: A New Ultraviolet Nonlinear Optical Material Derived from KBe2BO3F2 with High Performance and Excellent Water‐Resistance43A Sharp Improvement of Sulfate's Birefringence Induced by the Synergistic Effect of Heteroleptic and Dimeric Strategies14Advances in Solid-State Nonlinear Optical Materials: From Fundamentals to Applications61Multifunctional Chiral d 10 ‐Metal Coordination Polymers: Tunable Photoluminescence and Efficient Second‐Harmonic Generation with Circular Dichroic Response18Crystallography, Charge Transfer, and Two‐Photon Absorption Relations in Molecular Cocrystals for Two‐Photon Excited Fluorescence Imaging19C(NH2)3Cd(C2O4)Cl(H2O)·H2O and BaCd(C2O4)1.5Cl(H2O)2: Two Oxalate Chlorides Obtained by Chemical Scissors Strategy Exhibiting Low-Dimensional Structural Networks and Balanced Overall Optical Properties14Cd8(BO3)4SiO4: Metal Cation Inducing the Formation of Isolated [BO3] and [SiO4] Units in Borate Silicate15Fluorination strategy toward chemical and functional modification65Temperature-Induced Reversible Photoluminescence Switching and Ultraviolet-Pumped Light-Emitting Diode Applications of a Perovskite (C6H10N2)2MnCl6·2H2O Crystal26Secondary‐Bond‐Driven Construction of a Polar Material Exhibiting Strong Broad‐Spectrum Second‐Harmonic Generation and Large Birefringence41(C(NH2)3)2(I2O5F)(IO3)(H2O) and C(NH2)3IO2F2: Two Guanidine Fluorooxoiodates with Wide Band Gap and Large Birefringence20Nonlinear Optical Phosphide CuInSi2P4: The Inaugural Member of Diamond-Like Family I–III–IV2–V4 Inspired by ZnGeP216(C 3 N 6 H 7 )BF 4 ·H 2 O and (C 3 N 6 H 7 )SO 3 CH 3 ·H 2 O with large birefringence induced by coplanar π-conjugated [C 3 N 6 H 7 ] + groups33[(C 5 H 6 N 2 ) 2 H](Sb 4 F 13 ): a polyfluoroantimonite with a strong second harmonic generation effect60A bifunctional primitive strategy induces enhancements of large second harmonic generation and wide UV transmittance in rare-earth borates containing [B 5 O 10 ] groups22A UV non-hydrogen pure selenite nonlinear optical material for achieving balanced properties through framework-optimized structural transformation41Chemical modulation of A I RE III C IV QVI4 family compounds for band gap and optical anisotropy enhancement16Designing promising ultraviolet (UV) birefringent crystals with different hydrogen-bonded phosphate frameworks18Fully tricoordinated assembly unveils a pioneering nonlinear optical crystal (SbTeO 3 )(NO 3 )25Halide-driven polarity tuning and optimized SHG-bandgap balance in (C 4 H 11 N 2 )ZnX 3 (X = Cl, Br, I)34HgBr 2 : an easily growing wide-spectrum birefringent crystal38Hydrogen bonding bolstered head-to-tail ligation of functional chromophores in a 0D SbF 3 ·glycine adduct for a short-wave ultraviolet nonlinear optical material32KBa 3 M 2 F 14 Cl (M = Zr, Hf): novel short-wavelength mixed metal halides with the largest second-harmonic generation responses contributed by mixed functional moieties37Large optical anisotropy in noncentrosymmetric phosphate with pseudo 2D intercalated layer16Large second harmonic generation and birefringence from extended octupolar π-conjugated structures35New antimony fluorooxoborates with strong birefringence and unprecedented structural characterisation19Noncentrosymmetric tellurite halides created by a depolymerization strategy: toward strong SHG intensity and wide bandgap16Partial substitution with a significant effect: coexistence of a wide band gap and large birefringence in the oxychalcogenide AEGe 2 O 4 Se (AE = Sr and Ba)17Pb 2 (SeO 3 )(SiF 6 ): the first selenite fluorosilicate with a wide bandgap and large birefringence achieved through perfluorinated group modification45Recent advances in rational structure design for nonlinear optical crystals: leveraging advantageous templates153Research progress in optical materials with cationic organic planar π-conjugated groups containing CN bonds34Strategically designed metal-free deep-ultraviolet birefringent crystals with superior optical properties18Wide band gap selenide infrared nonlinear optical materials A II Mg 6 Ga 6 Se 16 with strong SHG responses and high laser-induced damage thresholds31Exceptional Optical Anisotropy Enhancement Achieved Through Dual‐Ions Cosubstitution Strategy in Novel Hybrid Bismuth Halides23KNa 2 Lu(BO 3 ) 2 : A Rare-Earth Borate Crystal Characterized by an Enhanced Birefringence and Wide Ultraviolet Transparency Range19Polysulfide Anions [S x ] 2− ( x = 2, 3, 4, 5): Promising Functional Building Units for Infrared Nonlinear Optical Materials22Molecular Crystals Constructed by Polar Molecular Cages: A Promising System for Exploring High‐performance Infrared Nonlinear Optical Crystals34Ultra-Broad-Band-Excitable Cu-Based Halide (C4H10N)4Cu4I8 with High Stability for LED Applications23Toward the ultraviolet (UV) or deep-UV nonlinear optical crystals: The combination of π-conjugated planar [XY3] and tetrahedral [XY4]80The Birefringence Modulation in Short‐Wave Ultraviolet Sulfates with Functional π‐Conjugated Cations and Polymerized Heteroleptic Tetrahedral Anions18Continuous-wave second-harmonic generation in the far-UVC pumped by a blue laser diode14Metal Methanesulfonates with Mixed Anionic Groups with Large Band Gaps and Enhanced Birefringence50[C(NH2)3][B(C2O2H4)2]: An Organic–Inorganic Hybrid Borate Containing Nonlinear-Optical Active Unit [B(C2O2H4)2]− with Solar-Blind-Region Optical Nonlinearity16Covalently bonded fluorine optimizing deep-ultraviolet nonlinear optical performance of fluorooxoborates56KPO2(NHCONH2)2: A Promising Deep-Ultraviolet Nonlinear Optical Phosphate Containing Polar [PO2(NHCONH2)2]− Tetrahedra15Hg4(Te2O5)(SO4): A Giant Birefringent Sulfate Crystal Triggered by a Highly Selective Cation153Trithionic guanidine: A novel semi-organic short-wave ultraviolet nonlinear optical sulfate with dimeric heteroleptic tetrahedra14Record Second-Harmonic Generation and Birefringence in an Ultraviolet Antimonate by Bond Engineering157UV-Transparent SHG Material Explored in an Alkali Metal Sulfate Selenite System16Theoretical Understanding of Nonlinear Optical Properties in Solids: A Perspective27A Noncentrosymmetric Metal‐Free Borophosphate: Achieving a Large Birefringence and Excellent Stability by Covalent‐Linkage27An Unprecedented [BO2]‐Based Deep‐Ultraviolet Transparent Nonlinear Optical Crystal by Superhalogen Substitution33Assembly of π‐Conjugated [B3O6] Units by Mer‐Isomer [YO3F3] Octahedra to Design a UV Nonlinear Optical Material, Cs2YB3O6F297Broadband Ultrafast Nonlinear Optical Limiting at a Porphyrin‐Based 2D Polymer14[Rb3BaCl][In8Se14]: Compressed chalcopyrite-type selenide achieved by polycationic substitution strategy toward excellent nonlinear optical property18A Chlorinated Indolium‐Based Nonlinear Optical Crystal Achieving Effective Terahertz‐Wave Generation and Highly Sensitive Detection19Structure‐Prediction‐Oriented Synthesis of Thiophosphates as Promising Infrared Nonlinear Optical Materials24Enhanced UV Nonlinear Optical Properties in Layered Germanous Phosphites through Functional Group Sequential Construction116[B3O3F4(OH)]2–: A Versatile Hydroxyfluorooxoborate Heteroanion Producing Compounds with Highly Tunable Optical Anisotropy19A3Sc(SO4)3 (A = K, Rb, Cs): Three Deep‐Ultraviolet Transparent Alkali‐Scandium Sulfates with Strong Second‐Harmonic Generation Response and High Thermal Stability14Tunable Intracavity Coherent Up‐Conversion with Giant Nonlinearity in a Polar Fluidic Medium16(C3N2H5)B3O3F2(OH)2: Realizing Large Birefringence via a Synergistic Effect between Anion F/OH‐Ratio Optimization and Cation Activation25The Directional Design of the Quasi‐Phase‐Matching Short‐Wave Ultraviolet Nonlinear Optical Crystal25Sulfate Derivatives with Heteroleptic Tetrahedra: New Deep‐Ultraviolet Birefringent Materials in which Weak Interactions Modulate Functional Module Ordering61Na2B6SO13 with unprecedented [B6SO13]∞ double chains and largest birefringence among borosulfates induced by the uniform arrangement of [B3O7] units19Functional Modules Map of Unexplored Chemical Space: Guiding the Discovery of Giant Birefringent Materials76Achieving the Birefringence Optimization by Methyl Modulation in Organic Nonlinear Optical Crystals15π-Lone pair synergy in (C7H4NO4)(IO3): Optimal balance among SHG, birefringence, and bandgap performance29Toward Strong UV–Vis–NIR Second-Harmonic Generation by Dimensionality Engineering of Zinc Thiocyanates32Nonlinear geometric phase coded ferroelectric nematic fluids for nonlinear soft-matter photonics81A Giant Optically Anisotropic Phosphate Driven by Mixed Valence Mercury Units22Enhanced Coplanarity and Giant Birefringence in Hydroxypyridinium Nitrate via Hydrogen Bonding between Planar Donors and Planar Acceptors15Enhanced Coplanarity and Giant Birefringence in Hydroxypyridinium Nitrate via Hydrogen Bonding between Planar Donors and Planar Acceptors53Chemical substitution towards a rare-earth borate ultraviolet NLO crystal exhibiting a strong SHG response17The New Paradigm of Ligand Substitution-Driven Enhancement of Anisotropy from SO4 Units in Short-Wavelength Region14Computer‐Aided Development of New Nonlinear Optical Materials38Dion–Jacobson Perovskites with a Ferroelectrically Switchable Chiral Nonlinear Optical Response57Breaking Performance Barriers in KBe 2 BO 3 F 2 (KBBF) Analogs by Functional Group Self‐Polymerization48Emergent Mid‐Infrared Nonlinear Optical Candidates With Targeted Balance Performances17Prismatic crystal field stabilized divalent rare-earth chalcogenide REIIBII6CIII6QVI16 with bifunctionality30Significant enhancement in the birefringence of metal phosphite halides via the introduction of π-conjugated cations17Hafnium-Based Chiral 2D Organic–Inorganic Hybrid Metal Halides: Engineering Polarity and Nonlinear Optical Properties via Para -Substituent Effects86AI2Mg3Ga12S22 (AI = K, Rb): T2-type supertetrahedra coupled with [MgS6] octahedra for designing wide-band gap infrared nonlinear optical materials with well-balanced properties16Designing Polar Covalent Hybrid Cadmium‐Based Chalcohalides Ultraviolet Nonlinear Optical Crystal with Strong Optical Anisotropy via Double‐Site Dual FBUs Tailoring25New Ways to Discover Novel Nonlinear Optical Materials: Scaling Machine Learning with Chemical Descriptors Information20[C 2 N 4 H 7 O][NH 2 SO 3 ]: High‐Performance Ultraviolet Nonlinear Optical Crystal with Ditrigon Coupled Guanylurea Group48A Wide Band Gap Germanate with the Largest Second Harmonic Generation Response Created by Hypoxic Strategy22From Holodirected to Hemidirected Coordination Activated by Oxygenation Strategy: A Facile Route to Long Wave Infrared Birefringent Crystal28Reinforced Nonlinear Optical Performances Induced by P‐P Homoatomic Bond in Phosphide SrIn 3 Si 4 P 1131(C6H10N2)ZnX4·H2O (X=Cl and Br): Excellent nonlinear optical properties and temperature induced photoluminescence for encryption23pH‐Dependent Switching Between Nonlinear‐Optical‐Active Nitrate‐Based Supramolecular Polymorphs27Rb 7 PbY 2 (B 5 O 10 ) 3 : A Noncentrosymmetric Rare-Earth Borate Nonlinear Optical Crystal with [B 5 O 10 ] Unit16Engineering an Excellent β ‐BaB 2 O 4 ‐Inspired UV Nonlinear Optical Material Through Secondary Building Unit Substitution21Expanding the Spectral Range in T2‐Supertetrahedral Nonlinear Optical Chalcogenides via Incorporating Inorganic Polycations29Ultra‐High Optical Anisotropy with UV Transmission Achieved by Rational Arrangement of Extended π‐Conjugated Groups46(3‐C6H10N2)ZnX4 (X = Cl and Br): Two Excellent UV Nonlinear Optical Crystals Designed by Combination of π‐conjugated and [ZnX4]2− Tetrahedral Units26Potassium Tetraiodatoiodate(III) Iodate(V): A Nonlinear Optical Crystal with Exceptional Second‐Harmonic Generation and Full‐Wavelength Phase Matching19Metal Cation Engineered UV Birefringent Crystals in π‐Conjugated Sulfonates with Record‐High Optical Anisotropy17Na[B3IO7(OH)] and Na2[B4IO9](IO3): Explorations of Boroiodates with Strong Second Harmonic Generation Response and Large Birefringence54Giant Birefringence Enabled by the Highly Anisotropic Linear IX 2 − (X = Cl, Br) Building Blocks32Bridging the Interlayer Binding to Ordered π‐Conjugated Units for Constructing High‐Performing Light Polarization Crystals48A transparent crystal with giant birefringence arising from π-electron anisotropy32Ca 7 (TeO 3 ) 6 (MoO 4 ): A Promising Mid-Infrared Nonlinear Optical Crystal Activated via a Module-Oriented Dimensionality Reduction Strategy34Decoupling the SHG‐Birefringence Trade‐off in UV NLO Materials via Triple‐Control Coordination Engineering: Achieving Synergistic Performance Optimization88[CON3H6BF4]: An Efficient Metal‐Free Borate with Optimized Birefringence Achieved by Structural Design Strategy15Giant Birefringence and Solar‐Blind Ultraviolet Transmission by Coordination‐Induced Assembly of π‐Conjugated Pyridine–Carboxylate24Simultaneous Boosting of Second Harmonic Generation and Circularly Polarized Luminescence in Chiral Hybrid Metal Halides Through Enhanced Octahedral Distortion27π‐Conjugated Cations in Phosphates: A Pathway to Solar‐Blind UV Nonlinear Optical Crystals with Phase‐Matching32Dual Chemical Scissors Strategy Enables 1D Antimony Selenates with Ultraviolet Nonlinear Optical Properties35Research progress and future prospect of chalcogenides with large optical anisotropy46Breaking the Birefringence Barrier in B–O Crystals via B–C π-scaffolding36CsICl 2 : A Record-Birefringent Inorganic Crystal with Ultrawide Infrared Transparency Enabled by Linear Interhalogen ICl 2 – Units36Rational Design of a Deep-Ultraviolet Nonlinear Optical Crystal25Sulfonated Module Aggregation for Ultrahigh Birefringence in Aqueous-Processable Crystals26Unlocking Advanced UV NLO Crystals in Rare‐Earth Metal Borate Fluorides via [B 3 O 6 ]‐Mediated Structural Modulation18[Hg3Se2]2- cluster drives giant optical anisotropy and broad infrared transparency16Functional Unit Design of Deep‐UV NLO Crystals With Short Phase‐Matching and Large SHG Response22Vacuum ultraviolet second-harmonic generation in NH4B4O6F crystal73Topology-Guided Discovery of BaIn 2 Si 7 P 12 : A Quaternary Diamond-like Framework Phosphide with Giant Second-Harmonic Generation and High Laser-Induced Damage Threshold22

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