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RESEARCH PAPER · Journal of the American Chemical Society · 2025

Hafnium-Based Chiral 2D Organic–Inorganic Hybrid Metal Halides: Engineering Polarity and Nonlinear Optical Properties via Para -Substituent Effects

Kyungmo Kim, Yang Li, Kang Min Ok

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Hafnium-Based Chiral 2D Organic–Inorganic Hybrid Metal Halides: Engineering Polarity and Nonlinear Optical Properties via Para -Substituent EffectsOriginalA five- and six-coordinated two-dimensional metal halide organic–inorganic phase transition material3Constructing a photoferroelectric semiconductor by regulating non-covalent interactions through halogen substitution7Dimensionality-driven photoluminescence enhancement in Cl/Br mixed-halide organic–inorganic hybrid cadmium halides3From poor-active to high performance via heteroleptic tetrahedra engineering: rational design of non-π-conjugated hybrids for phase-matchable ultraviolet nonlinear optics12Sb3+-Doped (TEA)2HfCl6 Metal Halide for White Light Emission and Anti-Counterfeiting Encryption0Stable zero-dimensional hybrid indium-based halides with yellow to orange light emission4Second-Harmonic Generation in Organic–Inorganic Hybrid Cadmium Thiocyanates Containing Terminal Amino Acids22Optical Investigation of a Non‐Centrosymmetric Tetrachlorocobaltate (II) Hybrid, in the Presence of Two Distinct Pyridine Molecules3Phase-Matching Second-Harmonic Generation in Zero-Dimensional Zinc Thiocyanates Ligated with Chiral Amino Acids6Reversible Solution–Gel–Crystal Transformations of Ethyltriphenylphosphonium Cuprous Iodide Single Crystals with Photo- and Radioluminescence2(CH5N3S)2Pb5Br10 and (CH5N3S)Pb2Br4: Two Nonlinear Optical Lead Thiosemicarbazide Bromides with Diverse Pb-Centered Building Units10Chiral Ligand-Induced Second-Harmonic Generation Response in Helical One-Dimensional Hybrid Lead Bromides9[Ga(C 2 H 6 OS) 6 ](SbBr 6 ): A Highly Luminescent Organic–Inorganic Hybrid Bimetallic Bromide Synthesized via a Cation Hybridization Strategy8π‐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‐Matching3Circularly Polarized Luminescence in Chiral Antimony(III) Chloride [Sb2Cl10]4– Dimers Induced by Asymmetric Hydrogen Bonding13Designing an all-organic wide bandgap ultraviolet nonlinear optical crystal3Exceptional Second Harmonic Generation in Ultraviolet Nonlinear Optical Oxyfluoroniobate Crystals via Structural Fingerprint Optimization of Polar Chains23Exceptional Second Harmonic Generation in Ultraviolet Nonlinear Optical Oxyfluoroniobate Crystals via Structural Fingerprint Optimization of Polar Chains8Eu(II) 4 Eu(III) 2 Ge 3 S 11 O 2 : a Single‐Element Mixed‐Valence Engineering Breakthrough for Strongly Enhanced Nonlinearity and Anisotropy in Rare‐Earth Oxysulfides8The birefringence optimization by hydroxyl in organic nonlinear optical crystals3Dimensional Engineering in Hybrid Transition Metal Halide Materials through the Introduction of Chiral Organic Cations5A Facile-Synthesized Cyan-Emitting Copper(I) Halide Hybrid Phosphor for 410 nm-Driven pc-WLEDs3Breaking 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 Incorporation4Organic Halogen Substitution-Driven Halogen Bonding Induces Polar 3D Supramolecular Framework and Second-Harmonic-Generation Response7Structural Transformation and Photochromism of Chiral Hybrid Metal Halides for Stimulus‐Responsive Phosphorescence and Circularly Polarized Luminescence5Structural Transformation and Photochromism of Chiral Hybrid Metal Halides for Stimulus‐Responsive Phosphorescence and Circularly Polarized Luminescence42Modulating Nonlinear Optical Performances in α/β-SnGa2GeS6 Polymorphs via Atomic Coordination Engineering1An Amide-Functionalized Pillar-Layered Metal–Organic Framework Based on Mixed Linker Systems with Enhanced Third-Order Nonlinear Optical Performance22Bright yellow emission from self-trapped exciton in a new antimony chloride-based hybrid material [C8H10N3]2SbCl53Chiral Metal Halides toward Circularly Polarized Photodetectors13Chiral‐Identified Multicolor‐Tunable Photoluminescence via Excitation‐Wavelength Modulation in 0D Antimony(III) Enantiomers for Multilevel Anti‐Counterfeiting10Structural Engineering for Chirality-Induced Spin Control in Metal–Halide Perovskites10Unlocking Strong Second‐Harmonic Generation in Deep‐UV‐Transparent Polar Organic Sulfonates through Connectivity Regulation2Unlocking Strong Second‐Harmonic Generation in Deep‐UV‐Transparent Polar Organic Sulfonates through Connectivity Regulation6Hydrogen‐Bond‐Driven Metal‐Free Crystal (C 6 H 7 N 2 O)(NH 2 SO 3 ) with Giant Birefringence and Solar‐Blind Ultraviolet Transmission0Phosphine Oxide-Metal Chelated Cuprous Iodide Hybrids with Rich Structural Architectures and Tunable Emission2Na2(C6H4NO3)2·H2O: A promising ultraviolet nonlinear optical crystal with strong second-harmonic generation effect and large birefringence1Chiral-Unit-Driven Short-Wave Ultraviolet Nonlinear Optical Acetates with Balanced Overall Optical Properties3Sb3 +‐Doped -doped (TEA)2HfCl6 metal halide for White Light Emissionwhite light emission and Anti‐Counterfeiting Encryptionanti-counterfeiting encryption1Lead‐Free Bandgap‐Engineered Perovskite with Thermally Activated SHG Switching and Enhanced X‐Ray Detection1Covalent hybrid cadmium halides with heteroleptic tetrahedral units exhibiting a wideband nonlinear optical response0Internally and externally induced chiral hybrid metal halide materials for advanced chiroptoelectronic applications23KGdSiSe 4 and KGdGeSe 4 : two rare earth-based selenides with wide bandgaps and large nonlinear optical responses0KGdSiSe4 and KGdGeSe4: Two Rare Earth Metal-Based Selenides with Wide Bandgaps and Large Nonlinear Optical Responses0Second-harmonic generation in two hybrid organic–inorganic metal chlorides based on l -thioproline ligand1Second-harmonic generation responses in low-dimensional metal bromides functionalized with l -arginine1Stable lead succinate-iodides with strong second-harmonic generation response and large birefringence0Suppressing antiparallel dipole alignment: A molecular engineering strategy toward sem-organic UV NLO crystals0Two hydrated ionic cocrystals of phenylphosphonate exhibiting second-harmonic generation and proton conductivity0The modulation of structural polarity facilitating the gradient enhancement of second harmonic generation effects in hybrid metal halides5Harnessing Reversible 0D–1D Transformation in Chiral Mn(II) Halides for Smart Circularly Polarized Luminescence Switching and Multi‐Level Encryption13Harnessing Reversible 0D–1D Transformation in Chiral Mn(II) Halides for Smart Circularly Polarized Luminescence Switching and Multi‐Level Encryption2Ligand-Isomerization Strategy Achieves Exceptional Wide-Range Zero-Thermal-Quenching Phosphorescence in Copper–Iodide Cluster–Organic Frameworks4Nonlinear Optical Responses in One-Dimensional Zinc Thiocyanates Functionalized with Natural Amino Acids8Topology-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 Threshold24C 6 H 7 NCl·X (X = Cl, Br): Outstanding Multifunctional Nonlinear Optical and Birefringent Crystals Enabled by Incorporation of π‐Conjugated Moieties2Application of Density Functional Theory for the Calculation of the Non‐Linear Optical Properties of Materials: A Comprehensive Review0Disentangling solvent effects on optical response via p-π and sp² lone-pair contributions in non-aromatic fused systems5(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 Conflicts14(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 Conflicts1Local Conformational Confinement and Dipole Engineering for Phase-Matchable Solar-Blind Ultraviolet Nonlinear Optical Crystals11Positional Isomerism Controls Polarity and Nonlinear Optical Properties in One‐Dimensional Hybrid Germanium Halides0Chiral (R/S‐MPz)Ge 4 I 10 With Unique 2D [Ge 4 I 10 ] Layered Structure and Large Chirality‐Induced Nonlinear Optical Effect0Second-harmonic generation circular dichroism of chiral organic–inorganic hybrid metal halides: Insights and perspectives2Zero-dimensional hybrid indium halides with broadband orange emission for white light emitting diodes0Engineering Multiple Hydrogen‐Bond Sites With D‐π‐A Motifs for Strong Optical Nonlinearity and Giant Birefringence in Organic‐Inorganic Halides4Engineering Multiple Hydrogen‐Bond Sites With D‐π‐A Motifs for Strong Optical Nonlinearity and Giant Birefringence in Organic‐Inorganic Halides1Advances in Imidazolate-Based Hybrid Organic–Inorganic Salts: Synthesis, Thermal, Conductivity, and Nonlinear Optical Responses0Amino Acid-Directed Synthesis of Chiral Manganese Chlorides with One-Dimensional Helical Structures0Research advances in rare-earth nonlinear optical crystalline materials in 20251Kinetic Trapping of Pressure‐Induced Symmetry Breaking in Hybrid Metal Halides via Fluorine‐Mediated Molecular Locking0Kinetic Trapping of Pressure‐Induced Symmetry Breaking in Hybrid Metal Halides via Fluorine‐Mediated Molecular Locking0Reversed Quantum‐Well Engineering Unlocks Large Ultraviolet Chiral Nonlinear Optical Response in a Water‐Resistant 2D Hybrid Fluorozirconate0Reversed Quantum‐Well Engineering Unlocks Large Ultraviolet Chiral Nonlinear Optical Response in a Water‐Resistant 2D Hybrid Fluorozirconate0Steric‐Guided Coordination Engineering Enables Significantly Optimized Optical Anisotropy via Sulfur‐Driven [C 5 H 5 NS] Birefringence‐Active Groups0Rational Design of a Strong Nonlinear Optical Crystal With Ultrawide Bandgap via Fine‐Tuning of Channel Structures0A Two‐Dimensional Organic Salt With a Deep‐Ultraviolet Cutoff Edge and Strong Second‐Harmonic Generation0A Two‐Dimensional Organic Salt With a Deep‐Ultraviolet Cutoff Edge and Strong Second‐Harmonic Generation0Local Aromatic Overlap Microregulation Enables Birefringence Enhancement in Isocompositional Hybrid Antimony Halides1HSAB‐Guided Design of Chiral Osmium Halides With Both Efficient Nonlinear Optical Properties and High Stability0HSAB‐Guided Design of Chiral Osmium Halides With Both Efficient Nonlinear Optical Properties and High Stability0An Excellent Deep‐Ultraviolet Nonlinear Optical Crystal Realized via a Functional Group Based on a Two‐in‐One Strategy0Halogen‐Bond Dimensionality Controls π–π Packing to Unlock Ultrahigh Second‐Harmonic Generation and Giant Birefringence0Halogen Substitution-Controlled Phase Transition, Dielectric Anomaly, and SHG Switching in Ga-Based Hybrid Molecular Ferroelectrics0

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  50. Suppressing antiparallel dipole alignment: A molecular engineering strategy toward sem-organic UV NLO crystals

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