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RESEARCH PAPER · Advanced Functional Materials · 2024

Functional Modules Map of Unexplored Chemical Space: Guiding the Discovery of Giant Birefringent Materials

Abudukadi Tudi, Zi‐Jian Li, Congwei Xie, Tuohetijiang Baiheti, Evgenii Tikhonov, Fangfang Zhang, Shilie Pan, Zhihua Yang

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Functional Modules Map of Unexplored Chemical Space: Guiding the Discovery of Giant Birefringent MaterialsOriginalExploring short-wavelength birefringent crystals via triggering cooperative arrangement between different π-conjugated groups8Modulating the birefringence of two-dimensional hybrid lead bromide perovskites using pyridine derivative cations11MgPO2F3: An Ultraviolet Nonlinear Optical System with an Extremely Short Phase-Matching Wavelength Achieved by Introducing Dual-Type Fluorine via Structure Prediction1Cation tuning in anionic framework hydroborates: tailored deep-ultraviolet optical crystals with large birefringence1Coordinated assembly of alkali and alkaline earth metals with the perfluorinated [AlF 6 ] group to design deep-ultraviolet zero-order waveplate materials2Exploring ultra-high optical anisotropy in polyiodides7Optimizing optical anisotropy in low-dimensional structures via intralayer hydrogen bonding modulation and anionic substitution17Structural chemistry of antimony( iii ) oxalates with lone pairs: polyhedral distortion [SbO 4 F 2 ], π-conjugation [C 2 O 4 ], and birefringence tuning1The impact of anionic group arrangement on the optical properties of the arsenate series0Can Low Structural Anisotropy Produce High Optical Anisotropy? Anomalous Giant Optical Birefringent Effect in PI4AlI4 in Focus11Chemical space as a unifying theme for chemistry20A Wide Band Gap Germanate with the Largest Second Harmonic Generation Response Created by Hypoxic Strategy22A Wide Band Gap Germanate with the Largest Second Harmonic Generation Response Created by Hypoxic Strategy5Na3Y2F3P2O8 and K4Y3F5P4O14: [YOF] Polyhedra Inducing Birefringence Enhancement in Non-π-Conjugated Phosphate Systems3From Holodirected to Hemidirected Coordination Activated by Oxygenation Strategy: A Facile Route to Long Wave Infrared Birefringent Crystal4From Holodirected to Hemidirected Coordination Activated by Oxygenation Strategy: A Facile Route to Long Wave Infrared Birefringent Crystal28The birefringence in orthorhombic and triclinic lead-iodates and the functional basic units' contribution: A first-principles investigation3K2PbB5P3O17: A Mixed-Coordinated Borophosphate with Enhanced Birefringence Driven by the [B2O5] Unit5Double Sb‐N Coordination Enables Record‐High Birefringence in UV‐Transparent Crystals71Double Sb‐N Coordination Enables Record‐High Birefringence in UV‐Transparent Crystals8Tuning Birefringence in Supramolecular Mg-PDA Frameworks: Modulating Bonding and Layer Connectivity0Designed Metal‐Free Quasi‐1D Crystals with Giant Birefringence8Metal Cation Engineered UV Birefringent Crystals in π‐Conjugated Sulfonates with Record‐High Optical Anisotropy17Unearthing Hydrogen Bonded Metal‐Free Crystal with Remarkable Optical Anisotropy9La2Zn3(SeO3)6: A UV Selenite Crystal with Second-Harmonic Generation and Large Birefringence13Improving the Performance of Birefringent Crystals by Molecular Assembly Strategy in the Solar‐Blind UV Region14Non-equivalent terminating roles of hydroxyl and fluorine in hydroxy/fluorooxo-borate optical functional materials2[TeSeS 2 ] 2− : The First Heterotriple‐Chalcogenide Motifs Decode Giant Mid‐Far Infrared Birefringence18[TeSeS 2 ] 2− : The First Heterotriple‐Chalcogenide Motifs Decode Giant Mid‐Far Infrared Birefringence4[C( NH2 )3] 2SiF6 : Design of Deep Ultraviolet Crystals with Large Birefringence Based on a Fluorination‐Oriented Strategy13Dual‐Sided Multidentate Coordination Strategy Enables Record Birefringence in UV‐Transparent Antimony‐Based Hybrid Crystals37Dual‐Sided Multidentate Coordination Strategy Enables Record Birefringence in UV‐Transparent Antimony‐Based Hybrid Crystals11Reversal Enhancement of Birefringence by Stereochemically Active Lone Pairs in Sn(II)-Based Mixed Halides0A strategy to achieve giant optical anisotropy via integrating linear pseudohalogen and stereochemical active lone pair cation6Optimizing the Hydrogen-Bond Network Drives Cadmium Ce(IV) Fluoride Hydrate with Significantly Enhanced Optical Anisotropy8(CN4H7)H2C3N3S3: Trithiocyanurate Exhibiting Giant Optical Anisotropy via Weak Interaction-Mediated Functional Module Alignment3Anion-Ordered [B3O5(OH)2] Induced by Crystal Water with Deep Ultraviolet Transparency and Large Birefringence in Boron-Rich Borophosphates4[C(NH2)3]Pb(C2O4)Cl·H2O: A halogen- and lone-pair-tuned UV crystal with large birefringence originated from cooperative π-conjugation6Five-Membered [C 5 O 5 ] 2 – Rings as Birefringence-Active Genes for Ultrabirefringent Crystals27Exceptional Enhancement of Optical Anisotropy Achieved via the Strategy of Combining Rigid Groups with High Symmetry and π‐Conjugated Organic Groups in Hybrid Fluorides33Triple Integration of π‐Conjugated Building Blocks: Unprecedented Assembly for Large Optical Anisotropy11Effect of Multiple Hydrogen Bonding on the π-Conjugated Groups and Optical Properties in Molecular Crystals5High‐Throughput Discovery of Large Birefringence Materials in Mixed‐N Hf‐O Systems0Achieving Ultra‐High Optical Anisotropy via Structural Regulation and Coplanar Engineering of Extended π‐Conjugated [H 2–x C 3 N 3 S 3 ] (x = 1, 2) Groups3[C(NH 2 ) 3 ] 2 PO 3 (OH): A Deep-Ultraviolet Birefringent Crystal Enabled by Synergy of π-Conjugated Cations and Heteroleptic Tetrahedra2LiV 3 Se 2 O 12 : A Promising Giant‐Birefringent Crystal Enabled by Significant Structural Distortion3Navigating the Landscape of Next-Generation Nonlinear Optical Materials Discovery: Opportunities and Challenges Driven by Artificial Intelligence4A 2 Sb 2 SO 4 F 6 (A = NH 4 + , Na + ): two sulfate fluoride crystals exhibiting enhanced birefringence driven by stereochemically active antimony( iii )1A multi-scale birefringence modulation strategy in DUV/UV crystals induced by organic cations1KTeOPO 4 and NH 4 SnClSO 4 : two new KTiOPO 4 derivatives as birefringent crystals featuring enhanced optical anisotropy0Na 2 SnSO 4 F 2 : an ultraviolet-transparent sulfate crystal with large birefringence driven by stereochemically active tin( ii )1Optimal three-dimensional [Ag 4 P 2 S 6 ]-framework assembly directed by a threefold roto-inversion axis for enhanced birefringence0Synergistic dual-modification strategy of π-conjugated cations and tetrahedra: rational design of ultraviolet high-birefringence monofluorophosphates0The condensation of π-conjugated units: a new paradigm for designing high-performance optical crystals4[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 Response22Overcoming the Bandgap‐Birefringence Trade‐Off: Proton‐Transfer Engineering of High‐Performance Ultraviolet‐Transparent Organic Crystal5Geometric Dilution and Electronic Confinement: Origin and Design of Giant Optical Anisotropy in Crystals with Layered Features1Hydrogen‐Bond‐Directed Assembly of Urea Derivatives: Exceptional Birefringence Achieved by π ‐Conjugated Unit Alignment3Electronegativity Adaption Approach for Solar‐Blind UV Birefringent Crystals With Ultrawide Bandgaps2Electronegativity Adaption Approach for Solar‐Blind UV Birefringent Crystals With Ultrawide Bandgaps1High‐Performance Infrared Nonlinear Optical Crystals Discovery Guided by High‐Throughput Computation, Machine Learning, and Experimental Verification6High‐Performance Infrared Nonlinear Optical Crystals Discovery Guided by High‐Throughput Computation, Machine Learning, and Experimental Verification2From Coplanarity to Coaxiality: A Linearity-Oriented Design Paradigm for Ultrahigh Ultraviolet Birefringent Inorganic Crystals4Steric hindrance and hydrogen-bond networks synergistically directing molecular alignment for high-performance ultraviolet birefringent1Achieving High‐Birefringence Thiophosphates From Low Polarizability Anisotropy Units by an Axial Linear Matching Strategy1Linear [ICl 2 ] Units Induced Giant Optical Anisotropy in AICl 2 (A = NH 4 , Rb): A Pathway to Advanced Birefringent Materials4Lock‐and‐Key Assembly Enables Record Birefringence in Monocyclic π‐Conjugated Crystals via Spatial Confinement of Linear Polyhalide5Lock‐and‐Key Assembly Enables Record Birefringence in Monocyclic π‐Conjugated Crystals via Spatial Confinement of Linear Polyhalide0Interlayer Electronic Decoupling Unlocks Giant Birefringence in π‐Conjugated Metal‐Organic Frameworks0Giant Birefringence and Ultrahigh Thermal Conductivity in Layered MgMoN 20Gravity‐Field Self‐Regulatory Engineering Enables PbIn 6 Te 10 Nonlinear Optical Crystals Boosting Laser‐Induced Damage Threshold1Toward the vacuum-ultraviolet frontier in nonlinear optical frequency conversion: phase-matching mechanisms across dimensions and architectures2Exceptional Solar‐Blind Birefringence Engineered by Complementary Hydrogen‐Bond Ordering of π‐Conjugated Units0Lateral‐Site Unblocking Enables Bilateral π ‐Chromophore Organization for Giant Birefringence in One‐Dimensional Lead Hybrids0Lateral‐Site Unblocking Enables Bilateral π ‐Chromophore Organization for Giant Birefringence in One‐Dimensional Lead Hybrids0

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  3. MgPO2F3: An Ultraviolet Nonlinear Optical System with an Extremely Short Phase-Matching Wavelength Achieved by Introducing Dual-Type Fluorine via Structure Prediction

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  4. Cation tuning in anionic framework hydroborates: tailored deep-ultraviolet optical crystals with large birefringence

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  5. Coordinated assembly of alkali and alkaline earth metals with the perfluorinated [AlF 6 ] group to design deep-ultraviolet zero-order waveplate materials

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  17. The birefringence in orthorhombic and triclinic lead-iodates and the functional basic units' contribution: A first-principles investigation

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