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RESEARCH PAPER · Angewandte Chemie International Edition · 2023

Fluorination Strategy Towards Symmetry Breaking of Boron‐centered Tetrahedron for Poly‐fluorinated Optical Crystals

Haotian Qiu, Fuming Li, Congcong Jin, Zhihua Yang, Junjie Li, Shilie Pan, Miriding Mutailipu

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Fluorination Strategy Towards Symmetry Breaking of Boron‐centered Tetrahedron for Poly‐fluorinated Optical CrystalsOriginalDiscovery of a new bimetallic borate with strong optical anisotropy activated by π-conjugated [B 2 O 5 ] units3Galloborates 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)34KBa 3 M 2 F 14 Cl (M = Zr, Hf): novel short-wavelength mixed metal halides with the largest second-harmonic generation responses contributed by mixed functional moieties37Magnesium cations as templates for the self-assembly of supramolecular luminescent {Mg@[B 18 φ 34–35 ]}-clusters0N-terminalized titanium carbide MXene coupled with graphene oxide toward optimized temporal domain-dependent nonlinear absorption9Pb 2 (SeO 3 )(SiF 6 ): the first selenite fluorosilicate with a wide bandgap and large birefringence achieved through perfluorinated group modification45Pb 3.5 GeS 4 Br 3 : the first phase-matching thiogermanate halide infrared nonlinear optical material12Pb 6 Ba 3 Si 2 S 8 I 10 : a new thiohalide with a quasi-two-dimensional structure and wide band gap2Strategically designed metal-free deep-ultraviolet birefringent crystals with superior optical properties18Wide band gap selenide infrared nonlinear optical materials A II Mg 6 Ga 6 Se 16 with strong SHG responses and high laser-induced damage thresholds31β -CsHg 2 I 5 , a compound with rare [Hg 2 I 5 ] dimers and large optical anisotropy2Synthesis, structures and properties of two new nitrate optical materials: Rb3ZnNO3Cl4 and Rb5Na(NO3)4Cl24Metal Methanesulfonates with Mixed Anionic Groups with Large Band Gaps and Enhanced Birefringence50Theoretical Investigation of Structural, Electronic and Optical Properties of Cs3MoO4(HCO3) with NLO Active Functional Units2From Cd(SCN) 2 (CH 4 N 2 S) 2 to Cd(SCN) 2 (C 4 H 6 N 2 ) 2 : Controlling Sulfur Content in Thiocyanate Systems Significantly Improves the Overall Performance of UV Nonlinear Optical Materials9From Cd(SCN) 2 (CH 4 N 2 S) 2 to Cd(SCN) 2 (C 4 H 6 N 2 ) 2 : Controlling Sulfur Content in Thiocyanate Systems Significantly Improves the Overall Performance of UV Nonlinear Optical Materials50(C8H6BrN2O)NO3: A Hybrid Nonlinear Optical Crystal With an Appropriate Birefringence12Improving the Electroluminescence Properties of New Chrysene Derivatives with High Color Purity for Deep-Blue OLEDs3Enhanced Birefringence in Phosphates via “Two Steps in One”: d0 Transition Metal Regulation and Fluorination Synergistic Strategy7Na3K6(CO3)3(NO3)2X·6H2O (X = NO3, Cl, Br): Exploring High-Performance UV Birefringent Crystals Induced by Coplanar π-Conjugated CO3 and NO3 Groups15NaRbB10O14(OH)4 and Na3CsB10O16(OH)2: Two Cases of Hydroxyborates with [B5Om(OH)n] Units and Deep Ultraviolet Cutoff Edges6Tunable Optical Anisotropy in Rare‐Earth Borates with Flexible [BO3] Clusters7Theoretical insight on structure, electronic, and optical properties of two d 0–d 10 electron transition-metal oxyhalides SHG materials2Mechanically deformable organic ferroelectric crystal with adaptive shape locking0Sulfate Derivatives with Heteroleptic Tetrahedra: New Deep‐Ultraviolet Birefringent Materials in which Weak Interactions Modulate Functional Module Ordering61Sulfate Derivatives with Heteroleptic Tetrahedra: New Deep‐Ultraviolet Birefringent Materials in which Weak Interactions Modulate Functional Module Ordering4Tetrahedra Modification of Phosphates for Optical Anisotropy Enhancement13Achieving the Birefringence Optimization by Methyl Modulation in Organic Nonlinear Optical Crystals15Constructing Ultraviolet Nonlinear Optical Crystals with Superior Thermal Stability Based on Organic π-Conjugated [HCOO] Groups6Carbonatoperoxovanadates with Strong Second‐Harmonic Generation: Insights from First‐Principles Calculations on Anisotropic Structures and Optical Parameters0The New Paradigm of Ligand Substitution-Driven Enhancement of Anisotropy from SO4 Units in Short-Wavelength Region14Looking Back the Nonlinear Optical Crystals in a Functionalized Unit's Perspective109La 3 (Ga 3 S 3 O 3 )(Si 2 O 7 ): An Oxychalcogenide Demonstrating Ultrawide Optical Bandgap and Favorable Birefringence Propelled by Divergent Anionic Groups6A new ultraviolet-transparent molybdate featuring a layered structure and moderate birefringence0A strongly birefringent sulfate crystal with a wide second-harmonic generation phase-matching range4Deep-ultraviolet sulfamate halides with halogen-centered secondary building units for enhanced optical anisotropy4K 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 birefringence2RbB 7 O 10 (OH) 2 and NaB 11 O 16 (OH) 2 : alkali metal hydroxyborates with two-dimensional layered structures and large birefringence1Two mixed P–O anionic phosphates with a distinctive structural transformation and deep ultraviolet cutoff edge0Pb9Si8O22Cl6 and Pb3.07Ca1.93Si3O11: Two Ultraviolet Nonlinear Optical Materials Exhibit a Moderate Second Harmonic Generation Response1BaFS: Birefringence Enhanced by the Transformation from Optical Isotropy to Anisotropy via Interlayer Anion Substitution8Zwitterionic Glycine-Based Antimony Fluorides with Exceptional Ultraviolet Nonlinear Optical Properties11AI2Mg3Ga12S22 (AI = K, Rb): T2-type supertetrahedra coupled with [MgS6] octahedra for designing wide-band gap infrared nonlinear optical materials with well-balanced properties16Inch‐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 Halides7Crystal Structures, Phase Transition, and Optical Properties of Two Rare Earth Borate Fluorides: α- and β-BaGdBO3F26Rb 7 PbY 2 (B 5 O 10 ) 3 : A Noncentrosymmetric Rare-Earth Borate Nonlinear Optical Crystal with [B 5 O 10 ] Unit16Mechanically deformable organic ferroelectric crystal with plasticity optimized by fluorination20Designed Metal‐Free Quasi‐1D Crystals with Giant Birefringence8Metal Cation Engineered UV Birefringent Crystals in π‐Conjugated Sulfonates with Record‐High Optical Anisotropy17Sb2(TeO4)(SO4): An Anhydrous Tellurite Sulfate with Large Birefringence and Enhanced Thermal Stability8Enhancement of optical anisotropy from [BF4] units by ligand substitution0Exceptional Second Harmonic Generation in Ultraviolet Nonlinear Optical Oxyfluoroniobate Crystals via Structural Fingerprint Optimization of Polar Chains22Exceptional Second Harmonic Generation in Ultraviolet Nonlinear Optical Oxyfluoroniobate Crystals via Structural Fingerprint Optimization of Polar Chains8Designing Hybrid Sb-Based Nonlinear Optical Crystals with Large Birefringence by Combining the Lone Pair and π-Conjugated Genes10Engineered Integration of Diverse Functional Units Induces Multifunctionality in Malonate‐Borate Hybrids44Research on Nonlinear Optical Materials Based on BO 3 and BO 4 Hydroxy Tetraborates4Growth, structure and optical properties of PbBi3PO8 crystals0Ba 3 (MoO 2 F 3 )PO 4 F 2 : Rational Design and Synthesis of an Alkaline-Earth Phosphate Fluoride as a Birefringent Crystal1Three new chiral schiff base crystals with naphthyl groups possess second harmonic generation: Experimental and theoretical investigations1ZnGa(SeO 3 ) 2 F: a UV transparent birefringent crystal explored in M( ii )–IIIA–selenite–F systems2A[N(SO 2 NH 2 ) 2 ] (A = Na, K, Rb, and Cs): enhancing birefringence of non π-conjugated deep-ultraviolet crystals via novel dimeric disulfonamide [N(SO 2 NH 2 ) 2 ] − groups0Effects of pressure on structural, electronic and optical properties of noncentrosymmetric monoclinic Na3Sr(PO4)(CO3) with discrete [PO4] and [CO3] units0K 7 MgY 2 (B 5 O 10 ) 3 : a novel ultraviolet nonlinear optical crystal based on the [B 5 O 10 ] functional unit2基于太赫兹光谱技术的硼酸氟化机理分析（特邀）0C 6 H 7 NCl·X (X = Cl, Br): Outstanding Multifunctional Nonlinear Optical and Birefringent Crystals Enabled by Incorporation of π‐Conjugated Moieties2Urea revisited: Isopropyl substitution for a balanced nonlinear optical performance0The Multi‐Scale Paradigm: An Integrated Design Logic for Nonlinear Optical Crystals1Dual‐Role BF 3 Anchoring Enables Giant Birefringence in Short‐Wave UV‐Transparent Fluoroborates0

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  1. Discovery of a new bimetallic borate with strong optical anisotropy activated by π-conjugated [B 2 O 5 ] units

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

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  3. Halide-driven polarity tuning and optimized SHG-bandgap balance in (C 4 H 11 N 2 )ZnX 3 (X = Cl, Br, I)

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    Jin Chen, Huai-Yu Wu, Miao‐Bin Xu, Mingchang Wang, Qianqian Chen, Bingxuan Li, Chun‐Li Hu, Ke‐Zhao Du

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  4. KBa 3 M 2 F 14 Cl (M = Zr, Hf): novel short-wavelength mixed metal halides with the largest second-harmonic generation responses contributed by mixed functional moieties

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    Mei Yan, Chun‐Li Hu, Ru‐Ling Tang, Wen‐Dong Yao, Wenlong Liu, Sheng‐Ping Guo

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  5. Magnesium cations as templates for the self-assembly of supramolecular luminescent {Mg@[B 18 φ 34–35 ]}-clusters

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    Sergey N. Volkov, Valentina A. Yukhno, A. M. Banaru, Dina V. Deyneko, Sergey M. Aksenov, Dmitri O. Charkin, Alexey V. Povolotskiy, Yevgeny E. Savchenko, Andrey A. Antonov, Maria Georgievna Krzhizhanovskaya, В. Л. Уголков, Vera A. Firsova, Yulia A. Vaitieva, Kirill N. Boldyrev, Р. С. Бубнова

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  6. N-terminalized titanium carbide MXene coupled with graphene oxide toward optimized temporal domain-dependent nonlinear absorption

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  7. Pb 2 (SeO 3 )(SiF 6 ): the first selenite fluorosilicate with a wide bandgap and large birefringence achieved through perfluorinated group modification

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    Pengfei Li, Chun‐Li Hu, Jiang‐Gao Mao, Fang Kong

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  8. Pb 3.5 GeS 4 Br 3 : the first phase-matching thiogermanate halide infrared nonlinear optical material

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  9. 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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  10. Strategically designed metal-free deep-ultraviolet birefringent crystals with superior optical properties

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  11. Wide band gap selenide infrared nonlinear optical materials A II Mg 6 Ga 6 Se 16 with strong SHG responses and high laser-induced damage thresholds

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  12. β -CsHg 2 I 5 , a compound with rare [Hg 2 I 5 ] dimers and large optical anisotropy

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  13. Synthesis, structures and properties of two new nitrate optical materials: Rb3ZnNO3Cl4 and Rb5Na(NO3)4Cl2

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  14. Metal Methanesulfonates with Mixed Anionic Groups with Large Band Gaps and Enhanced Birefringence

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  15. Theoretical Investigation of Structural, Electronic and Optical Properties of Cs3MoO4(HCO3) with NLO Active Functional Units

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  16. From Cd(SCN) 2 (CH 4 N 2 S) 2 to Cd(SCN) 2 (C 4 H 6 N 2 ) 2 : Controlling Sulfur Content in Thiocyanate Systems Significantly Improves the Overall Performance of UV Nonlinear Optical Materials

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  17. From Cd(SCN) 2 (CH 4 N 2 S) 2 to Cd(SCN) 2 (C 4 H 6 N 2 ) 2 : Controlling Sulfur Content in Thiocyanate Systems Significantly Improves the Overall Performance of UV Nonlinear Optical Materials

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  18. (C8H6BrN2O)NO3: A Hybrid Nonlinear Optical Crystal With an Appropriate Birefringence

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  19. Improving the Electroluminescence Properties of New Chrysene Derivatives with High Color Purity for Deep-Blue OLEDs

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  20. Enhanced Birefringence in Phosphates via “Two Steps in One”: d0 Transition Metal Regulation and Fluorination Synergistic Strategy

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  21. Na3K6(CO3)3(NO3)2X·6H2O (X = NO3, Cl, Br): Exploring High-Performance UV Birefringent Crystals Induced by Coplanar π-Conjugated CO3 and NO3 Groups

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  22. NaRbB10O14(OH)4 and Na3CsB10O16(OH)2: Two Cases of Hydroxyborates with [B5Om(OH)n] Units and Deep Ultraviolet Cutoff Edges

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  23. Tunable Optical Anisotropy in Rare‐Earth Borates with Flexible [BO3] Clusters

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  24. Theoretical insight on structure, electronic, and optical properties of two d 0–d 10 electron transition-metal oxyhalides SHG materials

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  25. Mechanically deformable organic ferroelectric crystal with adaptive shape locking

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  28. Tetrahedra Modification of Phosphates for Optical Anisotropy Enhancement

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  29. Achieving the Birefringence Optimization by Methyl Modulation in Organic Nonlinear Optical Crystals

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  30. Constructing Ultraviolet Nonlinear Optical Crystals with Superior Thermal Stability Based on Organic π-Conjugated [HCOO] Groups

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  31. Carbonatoperoxovanadates with Strong Second‐Harmonic Generation: Insights from First‐Principles Calculations on Anisotropic Structures and Optical Parameters

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  32. The New Paradigm of Ligand Substitution-Driven Enhancement of Anisotropy from SO4 Units in Short-Wavelength Region

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  33. Looking Back the Nonlinear Optical Crystals in a Functionalized Unit's Perspective

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  34. La 3 (Ga 3 S 3 O 3 )(Si 2 O 7 ): An Oxychalcogenide Demonstrating Ultrawide Optical Bandgap and Favorable Birefringence Propelled by Divergent Anionic Groups

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  35. A new ultraviolet-transparent molybdate featuring a layered structure and moderate birefringence

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  37. Deep-ultraviolet sulfamate halides with halogen-centered secondary building units for enhanced optical anisotropy

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  38. K 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 birefringence

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  39. RbB 7 O 10 (OH) 2 and NaB 11 O 16 (OH) 2 : alkali metal hydroxyborates with two-dimensional layered structures and large birefringence

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  40. Two mixed P–O anionic phosphates with a distinctive structural transformation and deep ultraviolet cutoff edge

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  41. Pb9Si8O22Cl6 and Pb3.07Ca1.93Si3O11: Two Ultraviolet Nonlinear Optical Materials Exhibit a Moderate Second Harmonic Generation Response

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  42. BaFS: Birefringence Enhanced by the Transformation from Optical Isotropy to Anisotropy via Interlayer Anion Substitution

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  43. Zwitterionic Glycine-Based Antimony Fluorides with Exceptional Ultraviolet Nonlinear Optical Properties

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  44. AI2Mg3Ga12S22 (AI = K, Rb): T2-type supertetrahedra coupled with [MgS6] octahedra for designing wide-band gap infrared nonlinear optical materials with well-balanced properties

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  45. Inch‐sized K[NH2(CH2COO)2]: a High‐Performance UV Nonlinear Optical Crystal Enabled by Novel Flexible π‐Conjugated Building Units, [NH2(CH2COO)2]−

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  48. Rb 7 PbY 2 (B 5 O 10 ) 3 : A Noncentrosymmetric Rare-Earth Borate Nonlinear Optical Crystal with [B 5 O 10 ] Unit

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  49. Mechanically deformable organic ferroelectric crystal with plasticity optimized by fluorination

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  50. Designed Metal‐Free Quasi‐1D Crystals with Giant Birefringence

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