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RESEARCH PAPER · ACS Materials Letters · 2022

Finding the First Squarates Nonlinear Optical Crystal NaHC4O4·H2O with Strong Second Harmonic Generation and Giant Birefringence

Xiaodong Zhang, Dong-Xu Cao, Daqing Yang, Ying Wang, Kui Wu, Ming‐Hsien Lee, Bingbing Zhang

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Finding the First Squarates Nonlinear Optical Crystal NaHC4O4·H2O with Strong Second Harmonic Generation and Giant BirefringenceOriginalK 2 S 4 O 6 : improving birefringence and nonlinear optical properties with the [O 3 S–S–S–SO 3 ] 2− group5Performance of optical materials with the derivative of planar π-conjugated groups: Recent advances and future prospects37Isotropically Dyed Single Crystals Produced via Gel-Incorporation20[Ba2F2][Ge2O3S2]: An Unprecedented Heteroanionic Infrared Nonlinear Optical Material Containing Three Typical Anions47KC9H5O6(H2O): A Promising UV Nonlinear-Optical Material with Large Birefringence Based on a π-Conjugated (C9H5O6)−Group11K 3 C 6 N 7 O 3 ·2H 2 O: A Multifunctional Nonlinear Optical Cyamelurate Crystal with Colossal π-Conjugated Orbitals44Na 2 (C 4 O 4 )(H 3 BO 3 )(H 2 O) 4 ·H 3 BO 3 : the first borate-squarate with strong SHG response obtained by superior synergy11Rb 3 B 11 P 2 O 23 : Materials Design of a New Chemically Benign Deep-Ultraviolet Nonlinear Optical Material58Deep-ultraviolet nonlinear-optical crystal BaNa2[PO3(OH)]2 with large birefringence and strong second-harmonic-generation response8High stability and moderate second-order nonlinear optical properties of hybrid lead-free perovskite [(CH 3 ) 3 NCH 2 Cl]CdCl 3 bulk crystals12Birefringence Regulation by Clarifying the Relationship Between Stereochemically Active Lone Pairs and Optical Anisotropy in Tin‐based Ternary Halides56Birefringence Regulation by Clarifying the Relationship Between Stereochemically Active Lone Pairs and Optical Anisotropy in Tin‐based Ternary Halides2Quadruple‐Bidentate Nitrate‐Ligated A 2 Hg(NO 3 ) 4 (A=K, Rb): Strong Second‐Harmonic Generation and Sufficient Birefringence59Quadruple‐Bidentate Nitrate‐Ligated A 2 Hg(NO 3 ) 4 (A=K, Rb): Strong Second‐Harmonic Generation and Sufficient Birefringence2NaCl·CH4N2O·H2O: An Organic–Inorganic Hybrid Ultraviolet Nonlinear Optical Crystal with Optimized Comprehensive Properties8Rational Design of Noncentrosymmetric Organic–Inorganic Hybrids with a π-Conjugated Pyridium-Type Cation for High Nonlinear-Optical Performance19K 2 RbB 8 PO 16 : A Borophosphate with Moderate Birefringence and Deep-Ultraviolet Transmission10A highly birefringent metal-free crystal assembled by cooperative non-covalent interactions30Ag 2 [TeO 2 (OH) 4 ]: a nonlinear optical tellurate with balanced comprehensive performance2Recent advances in rational structure design for nonlinear optical crystals: leveraging advantageous templates153Design of Deep-Ultraviolet Zero-Order Waveplate Materials by Rational Assembly of [AlO2F4] and [SO4] Groups9Two Acentric Zn-Based l -Tartrates with Moderate Second Harmonic Generation Responses and Large Birefringence6Homoatomic Polychalcogenide Nonlinear Optical Anionic Groups with Ultra-Large Optical Anisotropy31A solution-processable natural crystal with giant optical anisotropy for efficient manipulation of light polarization161Old tree blossoms anew: Research progress on the structures and optical properties of ultraviolet selenites56Breaking Boundaries: Giant Ultraviolet Birefringence in Dimension‐Reduced Zn‐Based Crystals66Breaking Boundaries: Giant Ultraviolet Birefringence in Dimension‐Reduced Zn‐Based Crystals8C6N7(NH2)3·H3PO4: Strong Second Harmonic Generation and Giant Birefringence Benefiting from Amino Substitution Strategy24Investigations of structure, thermal stability and optical properties of a new NLO crystal (C3H5N2)+(CF3COO)-0C2H12N6C4O4·2H2O and Na2C4O4·3H2O: Two Ultraviolet Birefringent Compounds with the [C4O4]2– Group3Constructing Ultraviolet Nonlinear Optical Crystals with Superior Thermal Stability Based on Organic π-Conjugated [HCOO] Groups6K4Cd3Ge4O13: A Congruent-Melting Germanate Nonlinear Optical Crystal with a Moderate Second-Harmonic Generation Intensity and Broad Transparent Window2Unveiling Noncentrosymmetric Pyridine Carboxylates from Centrosymmetric Templates through Motif Configuration Modulation in Zero-Dimensional System7Computer‐Aided Development of New Nonlinear Optical Materials38Computer‐Aided Development of New Nonlinear Optical Materials14Looking Back the Nonlinear Optical Crystals in a Functionalized Unit's Perspective109Advancements in squaric acid-based metal‒organic frameworks: transitioning from two-dimensional layers to three-dimensional networks0Enhanced second harmonic generation in a Fdd 2 polymorph of C 12 H 8 N 2 O 4 Zn for UV nonlinear optical applications1Greatly enhancing birefringence of fluorosilicates through the synergetic effect of functional units13Structural chemistry of antimony( iii ) oxalates with lone pairs: polyhedral distortion [SbO 4 F 2 ], π-conjugation [C 2 O 4 ], and birefringence tuning1Lithium Borate-Squarate: An Organic–Inorganic Groups-Mixed Nonlinear Optical Crystal with Large Birefringence4Two-Step Substitutions of Square Pyramidal VO5 with CdO4Br to Achieve Higher Laser-Induced Damage Threshold from Polar Oxybromides Rb4CdV5O15Br to Rb3CdV4O12Br10Designed Metal‐Free Quasi‐1D Crystals with Giant Birefringence8[CON3H6BF4]: An Efficient Metal‐Free Borate with Optimized Birefringence Achieved by Structural Design Strategy15Reversal Enhancement of Birefringence by Stereochemically Active Lone Pairs in Sn(II)-Based Mixed Halides0Achieving the birefringence-bandgap trade-off: Hydrogen-bond engineered biuret-cyanurate14Regulating the coplanarity of π-conjugated units through hydrogen bonding in FAHC2O4 and FAH2C3N3S3 crystals5Five-Membered [C 5 O 5 ] 2 – Rings as Birefringence-Active Genes for Ultrabirefringent Crystals27Remarkable Disparity of Second Harmonic Generation Response in Two Inorganic–Organic Hybrid Metal Thiocyanates5Achieving 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) Groups3Synergism of [C 2 N 4 H 7 S] cations and anionic modulators: tailoring second-order nonlinear optics and birefringence in organic–inorganic crystals6The Achievement of a Strong Second Harmonic Generation Response and a Large Birefringence in Sulfates4CdY 2 Si 2 S 8 : A Wide Bandgap IR NLO Material with d 10 Metal-Induced Structure Transformation from CS to NCS1Ultrawide Bandgap and Record-High Birefringence in a Covalent Beryllium-Organic Framework7Ordered Polar Topological Domains Enabling Giant Second‐Harmonic Generation in Ferroelectric Nematic Liquid Crystals0NaGa2PS6: A Noncentrosymmetric Thiophosphate with Wide Band Gap and High Laser-Induced Damage Threshold0

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  2. Performance of optical materials with the derivative of planar π-conjugated groups: Recent advances and future prospects

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  3. Isotropically Dyed Single Crystals Produced via Gel-Incorporation

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  4. [Ba2F2][Ge2O3S2]: An Unprecedented Heteroanionic Infrared Nonlinear Optical Material Containing Three Typical Anions

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  5. KC9H5O6(H2O): A Promising UV Nonlinear-Optical Material with Large Birefringence Based on a π-Conjugated (C9H5O6)−Group

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  6. K 3 C 6 N 7 O 3 ·2H 2 O: A Multifunctional Nonlinear Optical Cyamelurate Crystal with Colossal π-Conjugated Orbitals

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  7. Na 2 (C 4 O 4 )(H 3 BO 3 )(H 2 O) 4 ·H 3 BO 3 : the first borate-squarate with strong SHG response obtained by superior synergy

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  8. Rb 3 B 11 P 2 O 23 : Materials Design of a New Chemically Benign Deep-Ultraviolet Nonlinear Optical Material

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  9. Deep-ultraviolet nonlinear-optical crystal BaNa2[PO3(OH)]2 with large birefringence and strong second-harmonic-generation response

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  10. High stability and moderate second-order nonlinear optical properties of hybrid lead-free perovskite [(CH 3 ) 3 NCH 2 Cl]CdCl 3 bulk crystals

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  11. Birefringence Regulation by Clarifying the Relationship Between Stereochemically Active Lone Pairs and Optical Anisotropy in Tin‐based Ternary Halides

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  12. Birefringence Regulation by Clarifying the Relationship Between Stereochemically Active Lone Pairs and Optical Anisotropy in Tin‐based Ternary Halides

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  13. Quadruple‐Bidentate Nitrate‐Ligated A 2 Hg(NO 3 ) 4 (A=K, Rb): Strong Second‐Harmonic Generation and Sufficient Birefringence

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  14. Quadruple‐Bidentate Nitrate‐Ligated A 2 Hg(NO 3 ) 4 (A=K, Rb): Strong Second‐Harmonic Generation and Sufficient Birefringence

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  15. NaCl·CH4N2O·H2O: An Organic–Inorganic Hybrid Ultraviolet Nonlinear Optical Crystal with Optimized Comprehensive Properties

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  16. Rational Design of Noncentrosymmetric Organic–Inorganic Hybrids with a π-Conjugated Pyridium-Type Cation for High Nonlinear-Optical Performance

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  17. K 2 RbB 8 PO 16 : A Borophosphate with Moderate Birefringence and Deep-Ultraviolet Transmission

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  18. A highly birefringent metal-free crystal assembled by cooperative non-covalent interactions

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  19. Ag 2 [TeO 2 (OH) 4 ]: a nonlinear optical tellurate with balanced comprehensive performance

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

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  21. Design of Deep-Ultraviolet Zero-Order Waveplate Materials by Rational Assembly of [AlO2F4] and [SO4] Groups

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  22. Two Acentric Zn-Based l -Tartrates with Moderate Second Harmonic Generation Responses and Large Birefringence

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  23. Homoatomic Polychalcogenide Nonlinear Optical Anionic Groups with Ultra-Large Optical Anisotropy

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  24. A solution-processable natural crystal with giant optical anisotropy for efficient manipulation of light polarization

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  29. Investigations of structure, thermal stability and optical properties of a new NLO crystal (C3H5N2)+(CF3COO)-

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  30. C2H12N6C4O4·2H2O and Na2C4O4·3H2O: Two Ultraviolet Birefringent Compounds with the [C4O4]2– Group

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

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  32. K4Cd3Ge4O13: A Congruent-Melting Germanate Nonlinear Optical Crystal with a Moderate Second-Harmonic Generation Intensity and Broad Transparent Window

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  33. Unveiling Noncentrosymmetric Pyridine Carboxylates from Centrosymmetric Templates through Motif Configuration Modulation in Zero-Dimensional System

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  35. Computer‐Aided Development of New Nonlinear Optical Materials

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

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  37. Advancements in squaric acid-based metal‒organic frameworks: transitioning from two-dimensional layers to three-dimensional networks

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  38. Enhanced second harmonic generation in a Fdd 2 polymorph of C 12 H 8 N 2 O 4 Zn for UV nonlinear optical applications

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  42. Two-Step Substitutions of Square Pyramidal VO5 with CdO4Br to Achieve Higher Laser-Induced Damage Threshold from Polar Oxybromides Rb4CdV5O15Br to Rb3CdV4O12Br

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

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  44. [CON3H6BF4]: An Efficient Metal‐Free Borate with Optimized Birefringence Achieved by Structural Design Strategy

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  45. Reversal Enhancement of Birefringence by Stereochemically Active Lone Pairs in Sn(II)-Based Mixed Halides

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  46. Achieving the birefringence-bandgap trade-off: Hydrogen-bond engineered biuret-cyanurate

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  47. Regulating the coplanarity of π-conjugated units through hydrogen bonding in FAHC2O4 and FAH2C3N3S3 crystals

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  48. Five-Membered [C 5 O 5 ] 2 – Rings as Birefringence-Active Genes for Ultrabirefringent Crystals

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  49. Remarkable Disparity of Second Harmonic Generation Response in Two Inorganic–Organic Hybrid Metal Thiocyanates

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  50. Achieving 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) Groups

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