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RESEARCH PAPER · Chemical Society Reviews · 2023

Anisotropic structure building unit involving diverse chemical bonds: a new opportunity for high-performance second-order NLO materials

Xin Liu, Yi‐Chang Yang, Mengyue Li, Ling Chen, Li‐Ming Wu

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Anisotropic structure building unit involving diverse chemical bonds: a new opportunity for high-performance second-order NLO materialsOriginal[(C 5 H 6 N 2 ) 2 H](Sb 4 F 13 ): a polyfluoroantimonite with a strong second harmonic generation effect60[Sn 3 OF]PO 4 vs. [Sn 3 F 3 ]PO 4 : enhancing birefringence by breaking the R 3 symmetry and realigning lone pairs12A bifunctional primitive strategy induces enhancements of large second harmonic generation and wide UV transmittance in rare-earth borates containing [B 5 O 10 ] groups22Designing promising ultraviolet (UV) birefringent crystals with different hydrogen-bonded phosphate frameworks18Exploring a new short-wavelength nonlinear optical fluoride material featuring unprecedented polar cis -[Zr 6 F 34 ] 10− clusters48Galloborates 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)34Heteroanionic [VO x S 4− x ] groups: tetrahedral units with large birefringence for mid-infrared nonlinear optical crystals9Multi-fidelity machine learning for predicting bandgaps of nonlinear optical crystals14Pb 6 Ba 3 Si 2 S 8 I 10 : a new thiohalide with a quasi-two-dimensional structure and wide band gap2Rare-earth-based chalcogenides and their derivatives: an encouraging IR nonlinear optical material candidate70Recent advances in rational structure design for nonlinear optical crystals: leveraging advantageous templates153Reconstructing nearly isotropic microstructures to construct a one-dimensional framework causing record birefringence in thiophosphates13Sb4O5I2: Enhancing Birefringence through Optimization of Sb/I Ratio for Alignment of Stereochemically Active Lone Pairs18Exceptional Optical Anisotropy Enhancement Achieved Through Dual‐Ions Cosubstitution Strategy in Novel Hybrid Bismuth Halides23Enhancement of Birefringence in π-Conjugated Oxyfluorides Achieved via van der Waals Layered Structural Optimization10Two Hydroxyfluorooxoborates Achieving Deep‐Ultraviolet Cutoff Edges and Moderate Birefringence by Assembling Multi‐Anionic Groups6An Unprecedented [BO2]‐Based Deep‐Ultraviolet Transparent Nonlinear Optical Crystal by Superhalogen Substitution33An Unprecedented [BO2]‐Based Deep‐Ultraviolet Transparent Nonlinear Optical Crystal by Superhalogen Substitution1Theoretical Prediction of Monolayer BeP 2 O 4 H 4 with Excellent Nonlinear‐Optical Properties in Deep‐Ultraviolet Range6Breaking Boundaries: Giant Ultraviolet Birefringence in Dimension‐Reduced Zn‐Based Crystals66Breaking Boundaries: Giant Ultraviolet Birefringence in Dimension‐Reduced Zn‐Based Crystals8Recent advances and future perspectives on rare-earth-based nonlinear optical materials with π-conjugated [XO3] (X = B, C, N) units66Promising Functional Structural Building Unit Trisulfimide (SO2N)33– and Its Contributions to Second Harmonic Generation and Birefringence1C6N7(NH2)3·H3PO4: Strong Second Harmonic Generation and Giant Birefringence Benefiting from Amino Substitution Strategy24Realizing Excellent Infrared Nonlinear Optical Performance in Eu-Based Chalcogenides via Rational Cross Substitution Strategy26π-Lone pair synergy in (C7H4NO4)(IO3): Optimal balance among SHG, birefringence, and bandgap performance29Li2NaB3S2O12: A Deep-UV Transparent Borosulfate with Moderate Birefringence Derived from the [B3S2O12]∞ Infinite Chain Designed by the High Boron-to-Sulfur Ratio Strategy6Enhanced 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 Acceptors53[C3H7N6]3[B3O5(OH)2] and [C3H8N6]4[B12O19(OH)6]: Two Melamine Borates with Large Birefringence13Achieving Phase‐Matching in Nonlinear Optical Materials CsM 2 In 2 S 6 (M = Cd/In, Hg/In) by the Incorporation of Unprecedented Trigonal Planar MS 3 Motifs6Functional assembly and modification of nonlinear optical fundamental motifs in phosphates27Balanced IR Nonlinear Optical Performance Achieved by Cation–Anion Module Cosubstitution in V-Based Salt-Inclusion Oxychalcogenides22Computer‐Aided Development of New Nonlinear Optical Materials38Computer‐Aided Development of New Nonlinear Optical Materials14Looking Back the Nonlinear Optical Crystals in a Functionalized Unit's Perspective109Tin chalcohalide Sn 11 (PS 4 ) 4 I 10 obtained from structural-template-oriented synthesis: exhibiting balanced infrared nonlinear optical performance6Unprecedented Deep Ultraviolet (DUV) Birefringence in Fluorides Constructed from Linear π‐Group Anisotropic Structure Building Units29Unprecedented Deep Ultraviolet (DUV) Birefringence in Fluorides Constructed from Linear π‐Group Anisotropic Structure Building Units1Bulk crystal growth and optical properties of a novel organic–inorganic hybrid nonlinear optical thiocyanate: [Mn(CH 3 CONH 2 ) 2 ] [Hg(SCN) 4 ]10Cationic substitution engineering induces a new quaternary chalcogenide in the A–M IIIA –M IVA –Q system for optical crystal applications1Exploring new horizons in mid-to-far infrared nonlinear optical crystals: the significant potential of trigonal pyramidal [TeS 3 ] 2− functional units18Isovalent cation substitution drives structural transformation and infrared nonlinear optical activity in Eu-based chalcogenides11K 2 SO 4 (NH 3 SO 3 ) 2 and Cs 2 SO 4 (NH 3 SO 3 ) 3 : two deep-UV transparent sulfamate-sulfates with moderate birefringence2Prismatic crystal field stabilized divalent rare-earth chalcogenide REIIBII6CIII6QVI16 with bifunctionality30Search for New Members of the Abre(B15o30)N Family with Significant Shg Effects Based on Chemical Substitution Strategy0Structural diversity and photocurrent responses of multi-component chalcogenidometalates8Designing Polar Covalent Hybrid Cadmium‐Based Chalcohalides Ultraviolet Nonlinear Optical Crystal with Strong Optical Anisotropy via Double‐Site Dual FBUs Tailoring25Strong Second‐Harmonic Generation Responses in Salt‐Inclusion Oxychalcogenides Enabled by the Highly Distorted Polyhedra with Mixed‐Anions4Unveiling the Intrinsic Superior SHG Performance of Ce 4+ Fluoride Masked by Subtle Ce 3+ Impurity and Its Effective Removal13Unveiling the Intrinsic Superior SHG Performance of Ce4+ Fluoride Masked by Subtle Ce3+ Impurity and Its Effective Removal2Two-in-one: assembling hybrid supertetrahedra chromophores and achieving high-performance “hexagonal warriors” in nonlinear optical crystals6Chalcophosphates: A plentiful source of infrared nonlinear optical materials42Inch‐sized K[NH2(CH2COO)2]: a High‐Performance UV Nonlinear Optical Crystal Enabled by Novel Flexible π‐Conjugated Building Units, [NH2(CH2COO)2]−13Regulation of Refractive Index by Halogens in Two-Dimensional Layered Methylsulfonate Halides7Second-Harmonic Generation in Organic–Inorganic Hybrid Cadmium Thiocyanates Containing Terminal Amino Acids22(C6H10N2)ZnX4·H2O (X=Cl and Br): Excellent nonlinear optical properties and temperature induced photoluminescence for encryption23Engineering 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 Substitution6Synergically Assembling Advantageous Groups toward High‐Performance Infrared Nonlinear Optical Materials A II CdSiSe 4 (A II = Sr, Ba)40(3‐C6H10N2)ZnX4 (X = Cl and Br): Two Excellent UV Nonlinear Optical Crystals Designed by Combination of π‐conjugated and [ZnX4]2− Tetrahedral Units26Computational Insights into Structural, Optoelectronic and Charge Transfer Properties of Monocarbonyl Curcumin Derivatives for Biomedical and Photonic Applications5Phase-Matching Second-Harmonic Generation in Zero-Dimensional Zinc Thiocyanates Ligated with Chiral Amino Acids6Nonbonding 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 Properties26From AgHgI(SO4) to AgHg3I3.2Cl1.8(SO4): Symmetry Breaking of the Belousovite‐Type Topology by Mixed Halides to Achieve Strong Nonlinear Optical Effect14Recent progress in structural design strategies of high-birefringence optical crystals54Cation Equivalent Multisubstitution Realizing Structure Transformation and Balanced Nonlinear Optical Performance of Quaternary Eu-Based Chalcogenides8[C(NH2)3]Y(HCOO)4: Constructing 3D Framework for Guanidine-Based UV Nonlinear Optical Crystals with Good Performance8Giant Birefringence and Solar‐Blind Ultraviolet Transmission by Coordination‐Induced Assembly of π‐Conjugated Pyridine–Carboxylate8Giant Birefringence and Solar‐Blind Ultraviolet Transmission by Coordination‐Induced Assembly of π‐Conjugated Pyridine–Carboxylate24Machine Learning Prediction on Birefringence of Nonlinear Optical Crystals and Polymorphs with Different Birefringence Activities2Unravelling the impact of octahedral distortion and non-covalent interactions on the hyperpolarizabilities of Co(II) and Ni(II) coordination complexes with uridine nucleotide11Research progress and future prospect of chalcogenides with large optical anisotropy46Compositional Design Guides Property Control in A 2 M 2+ x Ti 1–( x /4) Q 4 Semiconductors6Reversal Enhancement of Birefringence by Stereochemically Active Lone Pairs in Sn(II)-Based Mixed Halides0Cation-modulated aligned arrangement of [B3O7] units in an unprecedented 2∞[B3O5] layer with remarkable birefringence10Structural Evolution of Hybrid Bismuth-Based Halides toward Enhanced Second-Harmonic Generation Response and Birefringence through Multisite Chemical Substitution7Achieving the birefringence-bandgap trade-off: Hydrogen-bond engineered biuret-cyanurate14Lewis Acidity‐Governed Ion Exchange and Record Birefringence in A′[Ag 3 (PO 3 F) 2 ]11Lewis Acidity‐Governed Ion Exchange and Record Birefringence in A′[Ag 3 (PO 3 F) 2 ]2Incorporation of Cu2+ within the ligand cavities of porphyrin-based MOFs for enhanced nonlinear optical performance2Structure-property relationships in IR nonlinear optical chalcogenides with stereochemically active lone pairs29Regulating the coplanarity of π-conjugated units through hydrogen bonding in FAHC2O4 and FAH2C3N3S3 crystals5[HgX 2 ] Linear Group Enabled Ultraviolet Birefringent Crystal RbHg 5 Br 11 with Strong Optical Anisotropy and Wide Bandgap12Breaking 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 Incorporation4Remarkable Disparity of Second Harmonic Generation Response in Two Inorganic–Organic Hybrid Metal Thiocyanates5Origin of second harmonic generation in noncentrosymmetric crystal structures containing lone pair electrons5Exploring second-order NLO activity in Imidazolium quinoline-2-carboxylate dihydrate (IQD): Synthesis, crystal engineering, spectral and DFT insights4[Pb(ptz)(OH)(H2O)]: A Hybrid Nonlinear Optical Crystal with Large Birefringence0LiPb 3 GeS 4 Cl 3 : Quasi‐T 2 ‐Supertetrahedral 3D Framework Enabling Superior Optical Performance14LiPb 3 GeS 4 Cl 3 : Quasi‐T 2 ‐Supertetrahedral 3D Framework Enabling Superior Optical Performance3Remarkable Birefringence Enhancement Enabled by π-Conjugated Cyanoguanidine Group Based on Anisotropic Molecule Coordination Approach8Structural, spectral, dielectric, and nonlinear optical properties of 2,4,6-Trinitrophenol with optical limiting behavior3Ce-centered polyhedral arrangement pattern and optical performance in Ce-based nonlinear optical materials3π-Conjugated unit bridge for giant second-harmonic generation and birefringence in hybrid materials with dual heteroleptic polyhedra5Recent achievements of d0 transition-metal-based oxyfluorides: Crystal chemistry and application in second-order NLO materials10Unlocking 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 Regulation6A high-performance IR nonlinear optical material Sr 3 MnGe 2 S 8 achieved via partial cation substitution-induced structural transformation2Maximizing the second-harmonic generation response via coordination-induced localization of nonbonding electrons12Exploring Second-Order Nonlinear Optical Performance in Oxyquinolinium 3-carboxypropanoate: A Combined Experimental and DFT Study1Structural Symmetry and Mixed‐anion Engineering in Halopnictides for Extraordinary Second‐Harmonic Generation6Structural Symmetry and Mixed‐anion Engineering in Halopnictides for Extraordinary Second‐Harmonic Generation3Asymmetry-driven organic–inorganic hybrid strategy for constructing structures with exceptional organofunctionalized B–O units2A Deep-Ultraviolet Transparent Nonlinear Optical Hydrogen-Bonded Organic Framework21Amino Acid Modification in One-Dimensional Cadmium Thiocyanates for Enhancing Second-Harmonic Generation Response2Cationic‐Dual‐Modulated Linear and V‐Shaped Birefringent‐Active Unit Generates Remarkable Birefringence6Breaking the SHG-stability trade-off in UV nonlinear optical materials by polar-layer-dense-locking4Charge-order-induced directional enhancement of non-diagonal second-order nonlinear optical tensor components2Chiral calcium thiocyanate hybrids: amino acid-enabled structural diversity and second-harmonic generation0KGdSiSe 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 Responses0LiPb3GeS4Br3：含孤对电子功能化超四面体的红外非线性光学晶体（特邀）0Recent advances in organic–inorganic hybrid materials for optical waveguides and regulation0Synergistic dual-modification strategy of π-conjugated cations and tetrahedra: rational design of ultraviolet high-birefringence monofluorophosphates0Tailoring linear and nonlinear optical properties of 2D Sc 2 C MXenes via surface termination modulation0The condensation of π-conjugated units: a new paradigm for designing high-performance optical crystals4van der Waals layered CuInP 2 S 6 as infrared nonlinear optical material1Realizing Phase‐Matching of Nonlinear Optical [ABa 3 Br 2 ][Ga 5 Se 10 ] (A = Cs, Rb, K, Na) Through Large Anisotropic Lattice Distortion6Realizing Phase‐Matching of Nonlinear Optical [ABa 3 Br 2 ][Ga 5 Se 10 ] (A = Cs, Rb, K, Na) Through Large Anisotropic Lattice Distortion11[CdCl 2 (4-Aminopyridine) 2 ] n : Synergistic Enhancement of Second-Harmonic Generation and Birefringence Enabled by a π-Conjugated Ligand for UV Nonlinear Optics5[Hg3Se2]2- cluster drives giant optical anisotropy and broad infrared transparency16Selenium-Based Molecular Cage Crystal β-P 4 Se 3 Br 2 : A Promising Candidate for Infrared Nonlinear Optical Applications1Unit Symmetry‐Breaking and Layered Linear Ordering Enabling Superior Short‐Wave Ultraviolet Birefringent Crystal8Unit Symmetry‐Breaking and Layered Linear Ordering Enabling Superior Short‐Wave Ultraviolet Birefringent Crystal2Strategic Oxygen‐Substitution in Perfluorinated Ce(IV) Coordination Frameworks Triggers Dual‐Wavelength Nonlinear Optical Materials With Exceptional Performances3Strategic Oxygen‐Substitution in Perfluorinated Ce(IV) Coordination Frameworks Triggers Dual‐Wavelength Nonlinear Optical Materials With Exceptional Performances32Zn 4 (BO 3 ) 2 (CO 2 CH 2 NH 2 ) 2 ·H 2 O: An Organic–Inorganic Hybridized KBe 2 BO 3 F 2 -like Ultraviolet Nonlinear Optical Crystal3Programmable Anisotropic in Diazapyrene Cocrystals With Birefringence Exceeding 1.27Programmable Anisotropic in Diazapyrene Cocrystals With Birefringence Exceeding 1.21Harnessing tetrahedral diversity: The path to superior diamond-like IR NLO crystals13RbLa(SO 4 ) 2 : A KBBF-like Deep-UV Transparent Rare Earth Sulfate with Strong SHG Response and High Thermal Stability Enabled by Multicomponent Structural Design2Unlocking Strong SHG Response and Large Birefringence in Hybrid Antimony Halides via a Three-in-One Strategy7Coordination Geometry-Directed Optical Anisotropy and Phase-Matched Nonlinear Optics in Chiral Metal–Organic Frameworks2Topology-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 Threshold22Significant Enhancement of Birefringence Resulting from the Introduction of [BO 2 (OH)] Groups into Borosulfates0Confinement π‐Conjugated Moiety Tailoring to Achieve Record Deep‐UV Nonlinearity in Sulfates0A Polar Cerium Iodate Ce 2 (IO 3 ) 6 (H 2 O) with a Strong Second-Harmonic Generation Response in Trivalent Ce-Based Materials1(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 Conflicts13(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 Conflicts1Chirality-driven polar lattice engineering for high-performance organic nonlinear optical crystals3Synergistic Enhancement of Optical Anisotropy in Nitrate Sulfamate for UV Applications: Role of Functional Group Alignment and Hydrogen Bond Network1The Power of Pnictogen Bond: As─As Linkages Drive Wide Bandgap, Strong NLO Response and Large Birefringence in SrGa 3 Si 4 As 115The Power of Pnictogen Bond: As─As Linkages Drive Wide Bandgap, Strong NLO Response and Large Birefringence in SrGa 3 Si 4 As 110Circumventing the Eg–SHG trade-off in selenides: Salt-inclusion [X4Br2][MGa4Se10] with concurrent large band gap and strong nonlinear optical response1Halogen‐Rich Design Strategy: Rational Synthesis of High‐Performance Tetrahedron‐Based Chalcohalides for Advanced Infrared Optical Materials2Halogen‐Rich Design Strategy: Rational Synthesis of High‐Performance Tetrahedron‐Based Chalcohalides for Advanced Infrared Optical Materials2

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  1. [(C 5 H 6 N 2 ) 2 H](Sb 4 F 13 ): a polyfluoroantimonite with a strong second harmonic generation effect

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  2. [Sn 3 OF]PO 4 vs. [Sn 3 F 3 ]PO 4 : enhancing birefringence by breaking the R 3 symmetry and realigning lone pairs

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  3. A bifunctional primitive strategy induces enhancements of large second harmonic generation and wide UV transmittance in rare-earth borates containing [B 5 O 10 ] groups

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    Shuaifeng Li, Weiming Li, Xiang Li, Guangsai Yang, Ning Ye, Zhanggui Hu, Yicheng Wu, Conggang Li

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  4. Designing promising ultraviolet (UV) birefringent crystals with different hydrogen-bonded phosphate frameworks

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  5. Exploring a new short-wavelength nonlinear optical fluoride material featuring unprecedented polar cis -[Zr 6 F 34 ] 10− clusters

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  6. Galloborates as ultraviolet nonlinear optical crystals: advances and perspectives

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  8. Heteroanionic [VO x S 4− x ] groups: tetrahedral units with large birefringence for mid-infrared nonlinear optical crystals

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  10. Pb 6 Ba 3 Si 2 S 8 I 10 : a new thiohalide with a quasi-two-dimensional structure and wide band gap

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  11. Rare-earth-based chalcogenides and their derivatives: an encouraging IR nonlinear optical material candidate

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  12. Recent advances in rational structure design for nonlinear optical crystals: leveraging advantageous templates

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  13. Reconstructing nearly isotropic microstructures to construct a one-dimensional framework causing record birefringence in thiophosphates

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  17. Two Hydroxyfluorooxoborates Achieving Deep‐Ultraviolet Cutoff Edges and Moderate Birefringence by Assembling Multi‐Anionic Groups

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  18. An Unprecedented [BO2]‐Based Deep‐Ultraviolet Transparent Nonlinear Optical Crystal by Superhalogen Substitution

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  19. An Unprecedented [BO2]‐Based Deep‐Ultraviolet Transparent Nonlinear Optical Crystal by Superhalogen Substitution

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  20. Theoretical Prediction of Monolayer BeP 2 O 4 H 4 with Excellent Nonlinear‐Optical Properties in Deep‐Ultraviolet Range

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  21. Breaking Boundaries: Giant Ultraviolet Birefringence in Dimension‐Reduced Zn‐Based Crystals

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  22. Breaking Boundaries: Giant Ultraviolet Birefringence in Dimension‐Reduced Zn‐Based Crystals

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  23. Recent advances and future perspectives on rare-earth-based nonlinear optical materials with π-conjugated [XO3] (X = B, C, N) units

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  24. Promising Functional Structural Building Unit Trisulfimide (SO2N)33– and Its Contributions to Second Harmonic Generation and Birefringence

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  26. Realizing Excellent Infrared Nonlinear Optical Performance in Eu-Based Chalcogenides via Rational Cross Substitution Strategy

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  28. Li2NaB3S2O12: A Deep-UV Transparent Borosulfate with Moderate Birefringence Derived from the [B3S2O12]∞ Infinite Chain Designed by the High Boron-to-Sulfur Ratio Strategy

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  30. Enhanced Coplanarity and Giant Birefringence in Hydroxypyridinium Nitrate via Hydrogen Bonding between Planar Donors and Planar Acceptors

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  31. [C3H7N6]3[B3O5(OH)2] and [C3H8N6]4[B12O19(OH)6]: Two Melamine Borates with Large Birefringence

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  32. Achieving Phase‐Matching in Nonlinear Optical Materials CsM 2 In 2 S 6 (M = Cd/In, Hg/In) by the Incorporation of Unprecedented Trigonal Planar MS 3 Motifs

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  33. Functional assembly and modification of nonlinear optical fundamental motifs in phosphates

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  34. Balanced IR Nonlinear Optical Performance Achieved by Cation–Anion Module Cosubstitution in V-Based Salt-Inclusion Oxychalcogenides

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  35. Computer‐Aided Development of New Nonlinear Optical Materials

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