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RESEARCH PAPER · Angewandte Chemie International Edition · 2023

Design of the Ionic Organic Nonlinear Optical Material NH 4 [LiC 3 H(CH 3 )O 4 ] with Ultrawide Band Gap and Moderate Birefringence

Haotian Tian, Chensheng Lin, Yuqiao Zhou, Xin Lei Zhao, Huixin Fan, Tao Yan, Ning Ye, Min Luo

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Design of the Ionic Organic Nonlinear Optical Material NH 4 [LiC 3 H(CH 3 )O 4 ] with Ultrawide Band Gap and Moderate BirefringenceOriginalA pair of ionic 1D Cu( ii ) chain enantiomers simultaneously displaying large second- and third-harmonic generation responses12A potassium lead 2-methylmalonate-iodide nonlinear optical crystal with strong second-harmonic generation response and large birefringence2New Functional Groups Design toward High Performance Ultraviolet Nonlinear Optical Materials95Mg(C 3 O 4 H 2 )(H 2 O) 2 : A New Ultraviolet Nonlinear Optical Material Derived from KBe 2 BO 3 F 2 with High Performance and Excellent Water‐Resistance7Mg(C3O4H2)(H2O)2: A New Ultraviolet Nonlinear Optical Material Derived from KBe2BO3F2 with High Performance and Excellent Water‐Resistance43Unveiling the optical, thermal and nonlinear behavior of guanidinium benzenesulfonate: A promising organic single crystal for NLO applications38K(NH4)Zn2(PO4)2: a Beryllium-Free Sr2Be2B2O7 Derivative with Enhanced Interlayer Connectivity7Large optical anisotropy in noncentrosymmetric phosphate with pseudo 2D intercalated layer16Optimized arrangement of non-π-conjugated PO 3 NH 3 units leads to enhanced ultraviolet optical nonlinearity in NaPO 3 NH 328Li+(3)Mg−: A new alkaline earthide with large nonlinear optical response0Synthesis and Characterization of Metal Iso-cyamelurate K0.5In0.5(H2C6N7O3)2·9H2O with Large Birefringence8KPO2(NHCONH2)2: A Promising Deep-Ultraviolet Nonlinear Optical Phosphate Containing Polar [PO2(NHCONH2)2]− Tetrahedra15Designing Strong Polarity and High Configurational Entropy Flexible Units toward Excellent Ultraviolet Nonlinear Optical Materials42HgC4H4O6: A mercury tartrate exhibits phase matchable second harmonic generation effect1Intramolecular Hydrogen Bonds Enhance Structure Coplanarity, Resulting in Significant Birefringence in Bridged-Bipyridine Halides7Homoatomic Polychalcogenide Nonlinear Optical Anionic Groups with Ultra-Large Optical Anisotropy31Enhanced UV Nonlinear Optical Properties in Layered Germanous Phosphites through Functional Group Sequential Construction11Enhanced UV Nonlinear Optical Properties in Layered Germanous Phosphites through Functional Group Sequential Construction116Exploration of deep UV-NLO responses of non-conjugated crystal systems by harnessing aprotic solvents: DFT vs experimental4Impressive nonlinear optical response of π-conjugated, photoluminescent soft nanoparticles in polymer matrix6Achieving the Birefringence Optimization by Methyl Modulation in Organic Nonlinear Optical Crystals15Nonlinear optical cyanurate crystals15Breaking Performance Barriers in KBe 2 BO 3 F 2 (KBBF) Analogs by Functional Group Self‐Polymerization5Breaking Performance Barriers in KBe 2 BO 3 F 2 (KBBF) Analogs by Functional Group Self‐Polymerization48An excellent ultraviolet nonlinear optical crystal derived from the polar methylphosphonate unit8Co-ligand tuning of MOF structural anisotropy for giant optical birefringence7Design and Synthesis of Two Sn-Centered Mixed Halide Crystals with Enhanced Birefringence8Sr2Zn(C3N3O3)2: An Alkaline Earth and d10 Transition Metal Based Ultraviolet Cyanurate with Large Birefringence6An alkali and rare earth metal mixed cyanurate KLa2(C3N3O3)2Cl with large birefringence: Synthesis and characterization2Chiral-Unit-Oriented Design of Non-π-Conjugated Noncentrosymmetric Phosphates with Short Absorption Edges4Inch‐sized K[NH2(CH2COO)2]: a High‐Performance UV Nonlinear Optical Crystal Enabled by Novel Flexible π‐Conjugated Building Units, [NH2(CH2COO)2]−13Toward the Strongest Nonlinear Optical Response and Largest Birefringence in Solvent‐Free Organic–Inorganic Metal Halides by Hydrogen Bond Engineering39Double Sb‐N Coordination Enables Record‐High Birefringence in UV‐Transparent Crystals71Double Sb‐N Coordination Enables Record‐High Birefringence in UV‐Transparent Crystals8Engineering an Excellent β ‐BaB 2 O 4 ‐Inspired UV Nonlinear Optical Material Through Secondary Building Unit Substitution21Engineering an Excellent β ‐BaB 2 O 4 ‐Inspired UV Nonlinear Optical Material Through Secondary Building Unit Substitution6LiAgCe2F10(H2O)2: Focusing on the Cation Size Effect to Reasonably Design a Nonlinear Optical Hydrated Cerium(IV) Fluoride10Structural Design and Characterization of NLO Crystals Containing Alkoxy Chalcone Derivatives with High SHG Efficiency5Hydrogen‐Bonded Assembly of Functional Units for Constructing Linear and Nonlinear Optical Crystals10π‐Conjugated Cations in Phosphates: A Pathway to Solar‐Blind UV Nonlinear Optical Crystals with Phase‐Matching32π‐Conjugated Cations in Phosphates: A Pathway to Solar‐Blind UV Nonlinear Optical Crystals with Phase‐Matching3The riddle of α-resorcinol revisited—New perspectives on “pocket-like” structure1Hydrogen‐Bond‐Directed Modular Assembly of Polar Chains for Rational Construction of UV Nonlinear Optical Crystals14Hydrogen‐Bond‐Directed Modular Assembly of Polar Chains for Rational Construction of UV Nonlinear Optical Crystals3Synergistic Design of UV Nonlinear Optical Crystals: Harnessing Flexible π-Conjugated Anions and Guanidinium Cations for Enhanced Performance4Vacancy-driven tetrahedral distortion leading to exceptional second harmonic generation3Breaking the Deep‐UV Transparency/Optical Nonlinearity Trade‐Off: Three‐Parameter Optimization in Oxyfluorides by Tailoring d 0 ‐Metal Incorporation10Breaking the Deep‐UV Transparency/Optical Nonlinearity Trade‐Off: Three‐Parameter Optimization in Oxyfluorides by Tailoring d 0 ‐Metal Incorporation4Exceptional Enhancement of Optical Anisotropy Achieved via the Strategy of Combining Rigid Groups with High Symmetry and π‐Conjugated Organic Groups in Hybrid Fluorides33Shape‐Topology‐Driven Design of Deep Ultraviolet Nonlinear Optical Crystals: Engineering [CH 3 PO 3 ]–Metal‐Oxo Layered Frameworks for Enhanced SHG, DUV Transparency3pH‐Regulated Ring‐Opening/Closing Transformation in Polyoxometalates Enables High‐Performance Nonlinear Optical Crystals1pH‐Regulated Ring‐Opening/Closing Transformation in Polyoxometalates Enables High‐Performance Nonlinear Optical Crystals13Chiral Lead-Oxyiodide Nonlinear Optical Crystals Constructed on l -Malate Groups5Asymmetry-driven organic–inorganic hybrid strategy for constructing structures with exceptional organofunctionalized B–O units2From centrosymmetric (C 4 H 8 N 5 )(SbF 4 ) to polar (C 4 H 7 N 4 O)(SbF 4 ): a new UV nonlinear optical material achieved by functional group modulation8Halide anion-mediated crystal structure engineering in guanidinoacetic acid halides for tunable birefringence0Regulating KBBF-like structures via a charge-assisted hydrogen-bonded framework to enable easily grown ultraviolet nonlinear optical crystals0Stable lead succinate-iodides with strong second-harmonic generation response and large birefringence0Truss bridge-like anhydrous stacking in hybrid crystals triggers ultra-high stability and robust birefringence0KHg 4 Ga 5 S 12 : A Diamond-like Tetrahedral Chalcogenide Exhibiting Giant Phase-Matching Second Harmonic Generation6C 6 H 7 NCl·X (X = Cl, Br): Outstanding Multifunctional Nonlinear Optical and Birefringent Crystals Enabled by Incorporation of π‐Conjugated Moieties2(C 5 H 7 N 2 ) (C 8 H 4 O 4 ) PbBr: Jahn–Teller Distortion‐Induced Tilting of π‐Conjugated Planes Resolving the Second‐Order Polarizability–Structural Anisotropy Conflicts13Anion Size‐Dependent Conformational Folding of Guanidinopropionate: Enabling Tunable Birefringence and Balanced Second‐Harmonic Generation Performance3Local Conformational Confinement and Dipole Engineering for Phase-Matchable Solar-Blind Ultraviolet Nonlinear Optical Crystals11Ultrawide Bandgap and Record-High Birefringence in a Covalent Beryllium-Organic Framework7Engineering Multiple Hydrogen‐Bond Sites With D‐π‐A Motifs for Strong Optical Nonlinearity and Giant Birefringence in Organic‐Inorganic Halides4Enhanced Birefringence in Organic–Inorganic Hybrid Antimony Halides via Partial Halogen Substitution1A Rigid‐Flexible Cooperative Bond‐Engineering Strategy for the Rational Design of Advanced Infrared Nonlinear Optical Crystals2Designing Novel Solar‐Blind Ultraviolet Nonlinear Optical Crystals Based on Local Proton Distribution Complementary Effect0A Two‐Dimensional Organic Salt With a Deep‐Ultraviolet Cutoff Edge and Strong Second‐Harmonic Generation0Laporte Selection Rule Induced the Suppression of d ‐ d Transitions and Vacancies Enhanced the Second Harmonic Generation in I 4¯‐MnGa 2 S 40The Parallel Coplanar Alignment of Planar Non‐π‐Conjugated [Pb 3 Br 3 ] Rings for a Stable Ultraviolet Nonlinear Optical Crystal0K3Sr3Li2Ga4B6O20F: A Sr2Be2B2O7-Type Ultraviolet Nonlinear Optical Crystal0Charge and structural flexibility of tartrate groups enable high-performance ultraviolet nonlinear optical crystals0Urea revisited: Isopropyl substitution for a balanced nonlinear optical performance0A novel tetrafluoroborate with giant birefringence assembled from biocompatible adenine0The Multi‐Scale Paradigm: An Integrated Design Logic for Nonlinear Optical Crystals1An Excellent Deep‐Ultraviolet Nonlinear Optical Crystal Realized via a Functional Group Based on a Two‐in‐One Strategy0Cation‐Regulated [CH 3 BO 2 F]‐Derived Borates: Synergistic Fluorination and Organic Functionalization for High‐Birefringence UV NLO Materials0

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  2. A potassium lead 2-methylmalonate-iodide nonlinear optical crystal with strong second-harmonic generation response and large birefringence

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  4. Mg(C 3 O 4 H 2 )(H 2 O) 2 : A New Ultraviolet Nonlinear Optical Material Derived from KBe 2 BO 3 F 2 with High Performance and Excellent Water‐Resistance

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  5. Mg(C3O4H2)(H2O)2: A New Ultraviolet Nonlinear Optical Material Derived from KBe2BO3F2 with High Performance and Excellent Water‐Resistance

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  6. Unveiling the optical, thermal and nonlinear behavior of guanidinium benzenesulfonate: A promising organic single crystal for NLO applications

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  7. K(NH4)Zn2(PO4)2: a Beryllium-Free Sr2Be2B2O7 Derivative with Enhanced Interlayer Connectivity

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  16. Homoatomic Polychalcogenide Nonlinear Optical Anionic Groups with Ultra-Large Optical Anisotropy

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  17. Enhanced UV Nonlinear Optical Properties in Layered Germanous Phosphites through Functional Group Sequential Construction

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  19. Exploration of deep UV-NLO responses of non-conjugated crystal systems by harnessing aprotic solvents: DFT vs experimental

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