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RESEARCH PAPER · Accounts of Chemical Research · 2022

Local Polarity-Induced Assembly of Second-Order Nonlinear Optical Materials

Yanqiang Li, Junhua Luo, Sangen Zhao

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Local Polarity-Induced Assembly of Second-Order Nonlinear Optical MaterialsOriginalA UV solar-blind nonlinear optical crystal with confined π-conjugated groups13Accurate design and synthesis of nonlinear optical crystals employing KBe2BO3F2 as structural template55An overview of Mg-based IR nonlinear optical materials22From H 12 C 4 N 2 CdI 4 to H 11 C 4 N 2 CdI 3 : a highly polarizable CdNI 3 tetrahedron induced a sharp enhancement of second harmonic generation response and birefringence50Melilite oxychalcogenide Sr 2 FeGe 2 OS 6 : a phase-matching IR nonlinear optical material realized by isomorphous substitution30Structure and optical property evolution in PbM(PO 4 )X (M = Zn, Sn; X = halogen): SHG effect and birefringence21Synthesis, structure and characterization of Cd 2 TeO 3 Cl 2 with unprecedented [Cd 2 O 6 Cl 4 ] octahedral dimers5Two pairs of chiral Yb III enantiomers presenting distinct NIR luminescence and circularly polarized luminescence performances with giant differences in second-harmonic generation responses20Visualizing the alignment of lone pair electrons in La 3 AsS 5 Br 2 and La 5 As 2 S 9 Cl 3 to form an acentric or centrosymmetric structure10Nonlinear Optical Glass‐Ceramic From a New Polar Phase‐Transition Organic‐Inorganic Hybrid Crystal11Nonlinear Optical Glass‐Ceramic From a New Polar Phase‐Transition Organic‐Inorganic Hybrid Crystal35Recent advances in non-π-conjugated nonlinear optical sulfates with deep-UV absorption edge53Flux growth of nonlinear optical crystal K3B6O10Br with high optical quality and its electro-optical property8ε-La(IO3)3: A Polar Iodate with High Thermal Stability and a Large Second-Harmonic-Generation Response Obtained by a Supercritical Hydrothermal Method8A BBO-like trithiocyanate with significantly enhanced birefringence and second-harmonic generation39A Hydrogen Bonded Supramolecular Framework Birefringent Crystal89A Hydrogen Bonded Supramolecular Framework Birefringent Crystal13Design of the Ionic Organic Nonlinear Optical Material NH 4 [LiC 3 H(CH 3 )O 4 ] with Ultrawide Band Gap and Moderate Birefringence79Design of the Ionic Organic Nonlinear Optical Material NH 4 [LiC 3 H(CH 3 )O 4 ] with Ultrawide Band Gap and Moderate Birefringence9Recent advances in IR nonlinear optical chalcogenides with well-balanced comprehensive performance56Electronic Structure Modulation of Nanographenes for Second Order Nonlinear Optical Molecular Materials3ACd 4 Ga 5 Te 12 (A = K, Rb, Cs): Tellurides with a Strong Nonlinear Optical Response and Purple Emission24LiGa(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 Threshold26Theoretical investigations on ternary defective diamond-like infrared nonlinear optical materials in Be-Ga-Se system18Enhancing second harmonic generation response in infrared nonlinear optical material through Pb substitution: A study of LiPbSiS compound2New 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‐Resistance43Secondary‐Bond‐Driven Construction of a Polar Material Exhibiting Strong Broad‐Spectrum Second‐Harmonic Generation and Large Birefringence9Secondary‐Bond‐Driven Construction of a Polar Material Exhibiting Strong Broad‐Spectrum Second‐Harmonic Generation and Large Birefringence41An organic–inorganic hybrid perovskite material [Me 3 NCMe 3 ]GaCl 4 exhibits a two-step off–on–off SHG response with a large temperature interval6Approach for quality deep-ultraviolet nonlinear optical crystals via a substitution strategy of channel species in zeolite3Designing promising ultraviolet (UV) birefringent crystals with different hydrogen-bonded phosphate frameworks18From NaGa(IO3)3F to NaGa(IO3)2F2 and NaGa(IO3)4: The Effects of Chemical Substitution between F– Anions and IO3– Groups on the Structures and Properties of Gallium Iodates13Galloborates as ultraviolet nonlinear optical crystals: advances and perspectives8Halide-driven polarity tuning and optimized SHG-bandgap balance in (C 4 H 11 N 2 )ZnX 3 (X = Cl, Br, I)34Hydrogen bonding bolstered head-to-tail ligation of functional chromophores in a 0D SbF 3 ·glycine adduct for a short-wave ultraviolet nonlinear optical material32Multi-step cation substitution facilitating the exploration of potential infrared nonlinear optical materials6Optimized arrangement of non-π-conjugated PO 3 NH 3 units leads to enhanced ultraviolet optical nonlinearity in NaPO 3 NH 328Two chiral Co III and Ni II complexes with identical ligands presenting different nonlinear optical responses4Two chiral Eu III and Sm III enantiomeric pairs with enantiopure N-donor ligands: showing strong third-harmonic generation and photoluminescence properties7Wide band gap selenide infrared nonlinear optical materials A II Mg 6 Ga 6 Se 16 with strong SHG responses and high laser-induced damage thresholds31Device Design for Multitask Graphene Electromagnetic Detection Based on Second Harmonic Generation89Nonlinear Optical Switching in a Tin-Based Multilayered Halide Perovskite Activated by Stereoactive Lone Pairs and Confined Rotators12Rational Design of Novel Promising Infrared Nonlinear Optical Materials: Structural Chemistry and Balanced Performances156Li13YGe4O16: A Mid-infrared Rare-Earth Germanate Nonlinear Optical Crystal Featuring a Broad Transmission Range and an Enlarged Band Gap10Record Second-Harmonic Generation and Birefringence in an Ultraviolet Antimonate by Bond Engineering157Three types of promising functional building units for designing metal halide nonlinear optical crystals20Combining rigid and deformable groups to construct a robust birefringent crystal for compact polarization components25Room-Temperature Phase Transition Material with Switchable Second-Order Nonlinear Optical Properties9Homoatomic 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 Construction116The First Discovery of Spherical Carborane Molecular Ferroelectric Crystals25The First Discovery of Spherical Carborane Molecular Ferroelectric Crystals3Additive-Assisted Forming High-Quality Thin Films of Sn–Oxo Cluster for Nanopatterning37Screening Strategy Identifies an Overlooked Deep‐Ultraviolet Transparent Nonlinear Optical Crystal3Screening Strategy Identifies an Overlooked Deep‐Ultraviolet Transparent Nonlinear Optical Crystal45Tetrahedra Modification of Phosphates for Optical Anisotropy Enhancement13Impressive nonlinear optical response of π-conjugated, photoluminescent soft nanoparticles in polymer matrix6Chiral mono- and dinuclear CoII and CuII enantiomeric pairs with distinct enantiopure N-donor ligands: Presenting highly enhanced third-harmonic generation responses6π-Lone pair synergy in (C7H4NO4)(IO3): Optimal balance among SHG, birefringence, and bandgap performance29Rational Design of Novel Polar Nonlinear Optical Materials in Alkali Metal Rare Earth Iodates5Elevating Nonlinear Optical Response Through D‐Electron Modulation in Metal–Organic Frameworks3Deep‐Ultraviolet Transparent Nonlinear Optical Phosphates: A New Alternative to Conventional Borates9Machine Learning Guided Discovery of Non‐Linear Optical Materials14Novel antimony-based mixed halides exhibiting an excellent SHG response and a broad transmission range20Li3[AlP2O7F(OH)](H2O)0.5 and A[Al2(PO4)2F(H2O)](A = K, Rb): Counter Cation Templates Derived Three Polar Alkaline Metal Fluoroaluminophosphates6K6NaCaRe2(B5O10)3 (Re = Y, Lu): Two NLO Compounds Exhibiting a Short Absorption Edge in the A7–xA’xAeRe2(B5O10)3 (x = 0, 1) Family4Tin chalcohalide Sn 11 (PS 4 ) 4 I 10 obtained from structural-template-oriented synthesis: exhibiting balanced infrared nonlinear optical performance6Evaluation of microscopic origins of optical responses: based on rigorous atomic space tessellating6Ca 2 La(MS 4 )(BS 3 ) (M = Ge/Si and Sn/Si): high-performance infrared nonlinear optical materials designed using an atomic site co-occupancy strategy9Harnessing the dual role of DMSO in the synthesis of SbOCl·DMSO: an excellent nonlinear optical crystal with unique 1D spiral chain10Impact of nuclear number on SHG and THG performances: a comparative study of chiral mono- and dinuclear Tb III complexes with identical organic ligands2Significant enhancement in the birefringence of metal phosphite halides via the introduction of π-conjugated cations17Thermo-mechanical control of second harmonic generation in a ferroelectric plastic crystal1Chiral-Unit-Oriented Design of Non-π-Conjugated Noncentrosymmetric Phosphates with Short Absorption Edges4The spin–orbit coupling induced stereochemical activity and nonlinear optical response in Pb2BO3X (X = Cl, Br, I)2Inch‐sized K[NH2(CH2COO)2]: a High‐Performance UV Nonlinear Optical Crystal Enabled by Novel Flexible π‐Conjugated Building Units, [NH2(CH2COO)2]−13Rational design of a high-efficiency lead halide organic-inorganic hybrid nonlinear optical switch via molecular engineering5Multifunctional chiral dinuclear DyIII enantiomeric pairs: showing single-molecule magnet behaviors with very strong third-harmonic generation responses5Nonbonding Electron Inversion‐Driven Structural Engineering: Synergistic Enhancement of Linear and Nonlinear Optical Properties3Nonbonding Electron Inversion‐Driven Structural Engineering: Synergistic Enhancement of Linear and Nonlinear Optical Properties26Designing a 3‐Hydroxypropane‐1‐Sulfonate Deep‐Ultraviolet Nonlinear Optical Crystal9Synergistic triple-site engineering in ABX-type hybrid halides for high-performance nonlinear optical crystals13Cation Equivalent Multisubstitution Realizing Structure Transformation and Balanced Nonlinear Optical Performance of Quaternary Eu-Based Chalcogenides8Two Chiral EuIII Enantiomeric Pairs with Significantly Enhanced Photophysical and Third-Harmonic Generation Performances through the Coordination Roles of Enantiopure Bi- and Tridentate N-Donors8Symmetry Breaking via Anion-Molecule Synergy: Fluorine and Crystalline Water Directed Construction of Noncentrosymmetric Sr(IO2F2)2·2H2O0Designing an all-organic wide bandgap ultraviolet nonlinear optical crystal3Theoretical study on the structure-NLO property of dithiophene ethylene derivatives1Structural Evolution of Hybrid Bismuth-Based Halides toward Enhanced Second-Harmonic Generation Response and Birefringence through Multisite Chemical Substitution7Preparation of laminated safety glass based on poly(vinyl butyral) blended with chromophore0From Centrosymmetric Eu 2 Ga 2 S 5 to Noncentrosymmetric EuMg 6 Ga 6 S 16 via Introduction of Distorted MgS 6 Octahedron: Featuring Wide Bandgap and Nonlinear Optical Activity3Borosilicates as deep-ultraviolet transparent nonlinear optical crystals: Structural motifs, performance limits and future directions9Structure-property relationships in IR nonlinear optical chalcogenides with stereochemically active lone pairs29Breaking 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 Incorporation4Ag3In3(SeO3)3(SO4)F4: A Sulfate Selenite Nonlinear Optical Material with a Wide Bandgap3Maximizing the second-harmonic generation response via coordination-induced localization of nonbonding electrons12Ultra-Large Nonlinear Optical Properties of Boron and Nitrogen Co-Doped Graphdiyne: The Role of the Alkalides1Cation regulation achieves symmetry breaking: from centrosymmetric M 2 Cs 2 B 10 O 17 (M = Na, K) to noncentrosymmetric Na 3 CsB 10 O 172Structural Symmetry and Mixed‐anion Engineering in Halopnictides for Extraordinary Second‐Harmonic Generation6Structural Symmetry and Mixed‐anion Engineering in Halopnictides for Extraordinary Second‐Harmonic Generation3A Deep-Ultraviolet Transparent Nonlinear Optical Hydrogen-Bonded Organic Framework21(C 4 H 8 N 5 )(PhPHO 2 )·H 2 O: a polar ionic cocrystal with strong second-harmonic generation and high birefringence0Halogen-ion-driven polymorphs for high-performance nonlinear optical crystalline materials3Multilevel Helical Cd-based Coordination Polymers with Significant Second NLO Response Constructed from Lactic Acid Derivatives0Simultaneously switching both the magnetic behaviors and nonlinear optical processes in mononuclear DyIII complexes0立体化学活性孤对电子与极性基元协同构筑高性能紫外非线性光学晶体（NH4）2Sb3F9SeO4（特邀）0[CdCl 2 (4-Aminopyridine) 2 ] n : Synergistic Enhancement of Second-Harmonic Generation and Birefringence Enabled by a π-Conjugated Ligand for UV Nonlinear Optics51D Cobalt‐Cytidine Monophosphate Coordination Polymer Exhibiting Efficient Ultraviolet Second‐Harmonic Generation7Simultaneously switching both the magnetic behavior and nonlinear optical process in mononuclear DyIII complexes via the coordination role of enantiopure N3-pincers2K 3 YGe 3 O 9 : A Rare-Earth Germanate Nonlinear Optical Crystal with a Short Ultraviolet Cutoff Edge and Moderate Second-Harmonic Generation Response1Hydrogen-Bond-Directed Assembly of an Intramolecular Charge-Transfer Compound for Second-Order Nonlinear Optics1Enantiomeric Cd-based coordination polymers with multilevel helical structures and significant second NLO response constructed from lactic acid derivatives2Tuning linear and nonlinear optical performances of two eight- and nine-coordinated chiral SmIII enantiomeric pairs by enantiopure N-donor ligands1Regulating B‐O Arrangement Boosts Anisotropy in a Simple Rubidium Borate, Leading to a High‐Performance UV NLO Crystal0Metal–organic framework-based second-order nonlinear optical materials: From structural design to functional applications0Unlocking Nonlinear Optics and Photoluminescence with Simultaneous Enhancement of Bandgap and Birefringence in Hybrid Sb-Based Halides2Cation-driven symmetry breaking in rare-earth borates toward ultraviolet nonlinear optical materials1Tuning Second‐Order Nonlinear Optical Properties via Electronic Interaction Engineering: Distinct Roles of Nonconjugation, σ–π Conjugation, and Intramolecular Charge Transfer in Chalcogen‑Functionalized Closo ‐Carborane Hybrids0Advances in metal selenite nonlinear optical materials: halogens directed structure modulation and property optimization0[CN4H8]SiF6: Fluorination-guided design of deep-UV crystal with large birefringence0Polar Superstructure Electronics and Optoelectronics0Chiral dinuclear EuIII enantiomeric pairs: simultaneously showing photoluminescences, circularly polarized luminescences, second- and third-harmonic generations with enhanced performances0A Hydrogen-Bonded Molecular Crystal with Strong Optical Anisotropy and Large Second-Harmonic Generation Response0

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