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RESEARCH PAPER · ACS Central Science · 2022

Exploring Short-Wavelength Phase-Matching Nonlinear Optical Crystals by Employing KBe2BO3F2 as the Template

Zi‐Jian Li, Wenqi Jin, Fangfang Zhang, Zhihua Yang, Shilie Pan

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Exploring Short-Wavelength Phase-Matching Nonlinear Optical Crystals by Employing KBe2BO3F2 as the TemplateOriginalDramatically improved optical anisotropy by realizing stereochemically active lone pairs in a sulfate system, K 2 SO 4 ·HIO 323Enhancement of birefringence and refractive index dispersion optimization from iodates to fluorooxoiodates1K 5 [B 3 O 3 F 4 (OH)] 2 (NO 3 ): the first hydroxyfluorooxoborate-nitrate with a short ultraviolet cutoff edge and large birefringence18Linear π-conjugated units of the D ∞h point group as superior ultraviolet birefringent units1Mg 2 Pb 2 Si 2 O 7 F 2 : a new lead-containing alkali earth metal silicate fluoride with a short cutoff edge2Recent progress in borate-based short-wavelength nonlinear optical crystals with boron–oxygen skeleton modification28Synthesis and characterization of Cs 2 Zn 4 V 4 O 15 —a new vanadate in the Cs–Zn–V–O quaternary system5Synthesis, structures and properties of two new selenite optical materials: K 2 Zn 3 Se 4 O 12 and K 4 Zn 3 V 4 Se 2 O 192BaB2P2O8F2: A Fluoroborophosphate with [B2P2O8F2]∞ Layers and Deep-Ultraviolet Cutoff Edge4Ba2B9O13F4·BF4: first fluorooxoborate with unprecedented infinite [B18O26F8] tubes and deep-ultraviolet cutoff edge14Recent Development of Sn II , Sb III ‐based Birefringent Material: Crystal Chemistry and Investigation of Birefringence130Recent Development of SnII, SbIII‐based Birefringent Material: Crystal Chemistry and Investigation of Birefringence6Na2BaB12O18F4: A Mixed Alkali/Alkaline-Earth Metal Fluorooxoborate with Two Unprecedented Interpenetrating Three-Dimensional B–O/F Anionic Networks and a Short Ultraviolet Cutoff Edge9Theoretical Prediction‐Assisted Synthesis and Characterization of Infrared Nonlinear Optical Material NaSrBS324Cs 3 [(BOP) 2 (B 3 O 7 ) 3 ]: A Deep-Ultraviolet Nonlinear Optical Crystal Designed by Optimizing Matching of Cation and Anion Groups169Hg3(SeO3)2(SO4): A UV Nonlinear Optical Mercury Selenite Sulfate Constructed by Neat [Hg6O8(SeO3)4]∞ Layers and SO4 Tetrahedra27Target-Oriented Synthesis of Borate Derivatives Featuring Isolated [B3O3] Six-Membered Rings as Structural Features20Ultraviolet Crystal with Strong Optical Nonlinearity by Creating Halogen-Centered Secondary Building Blocks15A survey of stereoactive oxysalts for linear and nonlinear optical applications40Three Borates Belonging to the A(I)7Ae(II)Re(III)2B15O30 Family as Promising Nonlinear Optical Crystals12Binary Heterogroup-Templated Scaffolds of Polyoxopalladates as Precatalysts for Plasma-Assisted Ammonia Synthesis13Sr(NO 3 )(NH 2 SO 3 )·H 2 O: First Nitrate Sulfamate Revealing Remarkable Second Harmonic Generation and Optimized Birefringence25Na 6 Mg 3 P 4 S 16 and RbMg 2 PS 4 Cl 2 : two Mg-based thiophosphates with ultrawide bandgaps resulting from [MgS 6 ] and [MgS x Cl 6− x ] octahedra4A2Hgx(SeO3)y (A = K, Rb, Cs): Three Alkali Metal Mercury Selenites Featuring Unique 1D [HgOm(SeO3)n]∞ Chains13K 2 RbB 8 PO 16 : A Borophosphate with Moderate Birefringence and Deep-Ultraviolet Transmission10Cd8(BO3)4SiO4: Metal Cation Inducing the Formation of Isolated [BO3] and [SiO4] Units in Borate Silicate15“One stone two birds” design of borates featuring edge-sharing [BO 4 ] and different B–O configurations in one structure utilizing covalent tetrahedra8CsAlB 3 O 6 Cl: the rational construction of a KBBF-type structure with aligned 2 ∞ [AlB 3 O 6 Cl] layers via introducing unprecedented [AlO 3 Cl] tetrahedra5Exploration of antimony( iii ) oxyhalides via single-site substitution in quest of large birefringence10K, Rb-hydroxyborates series with deep-ultraviolet KRbB 5 O 8 (OH) possessing moderate second harmonic generation response0NaB(OH) 3 CH 3 : a deep-ultraviolet optical crystal with unprecedented methyl-modified [B(OH) 3 CH 3 ] units6Recent advances in rational structure design for nonlinear optical crystals: leveraging advantageous templates153Structural characterisation and optical properties of new alkaline earth phosphate CaMg(P 4 O 12 ) and alkaline alumophosphate Cs 3 Al 4 (PO 4 ) 51新型深紫外非线性光学晶体研究进展（特邀）9Toward the ultraviolet (UV) or deep-UV nonlinear optical crystals: The combination of π-conjugated planar [XY3] and tetrahedral [XY4]80AYSO4F2 (A = K, Rb): [YO4F4] Polyhedra Enhancement of Birefringence in Non-π-Conjugated Sulfate Systems9A perspective on deep-ultraviolet nonlinear optical materials13Two Hydroxyfluorooxoborates Achieving Deep‐Ultraviolet Cutoff Edges and Moderate Birefringence by Assembling Multi‐Anionic Groups6NaRbB10O14(OH)4 and Na3CsB10O16(OH)2: Two Cases of Hydroxyborates with [B5Om(OH)n] Units and Deep Ultraviolet Cutoff Edges6Structure‐Prediction‐Oriented Synthesis of Thiophosphates as Promising Infrared Nonlinear Optical Materials24Structure‐Prediction‐Oriented Synthesis of Thiophosphates as Promising Infrared Nonlinear Optical Materials1Enhanced UV Nonlinear Optical Properties in Layered Germanous Phosphites through Functional Group Sequential Construction11Enhanced UV Nonlinear Optical Properties in Layered Germanous Phosphites through Functional Group Sequential Construction116Fluorine-driven materials design of novel deep-ultraviolet nonlinear optical crystal materials: Research progress and challenges6A3Sc(SO4)3 (A = K, Rb, Cs): Three Deep‐Ultraviolet Transparent Alkali‐Scandium Sulfates with Strong Second‐Harmonic Generation Response and High Thermal Stability14NH4Y(SO4)2·H2O and NH4YSO4F2: Two New Ammonium‐Rare Earth Metal Sulfates with Enhanced Optical Anisotropy and Deep Ultraviolet Transmission3Tunable Intracavity Coherent Up‐Conversion with Giant Nonlinearity in a Polar Fluidic Medium16The Directional Design of the Quasi‐Phase‐Matching Short‐Wave Ultraviolet Nonlinear Optical Crystal25Sulfate 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 Ordering4Li2NaB3S2O12: A Deep-UV Transparent Borosulfate with Moderate Birefringence Derived from the [B3S2O12]∞ Infinite Chain Designed by the High Boron-to-Sulfur Ratio Strategy6Learning From Nature: The Rational Non‐Centrosymmetric Structural Design in the Honeycomb‐Like Gaudefroyite Family23Rb 1.87 Cs 1.13 B 8 O 13 (NO 3 ): a new acentric borate-nitrate with two types of three-dimensional interpenetrating lattices1Structural Evolution and Optical Properties of Hydroxyfluorooxoborates MM′2n-1[B3O3F4(OH)]n (M = K, Cs, and Rb; M′ = K, NH4, and Cs; n = 1, 2, and 3)12MgPO2F3: An Ultraviolet Nonlinear Optical System with an Extremely Short Phase-Matching Wavelength Achieved by Introducing Dual-Type Fluorine via Structure Prediction1A remarkable solar-blind ultraviolet nonlinear optical crystal with comprehensive performance and enhanced thermal stability4A strongly birefringent sulfate crystal with a wide second-harmonic generation phase-matching range4An excellent ultraviolet nonlinear optical crystal derived from the polar methylphosphonate unit8BaAlPO 4 F 2 : structure and properties of the first barium fluoroaluminophosphate with the mixed anion group [Al 2 PO 8 F 5 ]1CsBO(OH) 2 : a new hydroxyborate with the rare [BO(OH) 2 ] group and a deep ultraviolet cutoff edge3Expanding silver fluorooxoborate crystal chemistry: Ag 2 B 5 O 8 F with 3D double interpenetrating frameworks and Ag 3 B 5 O 8 F 2 with 2D layers5Exploring quaternary vanadates containing alkali metals, alkaline earth metals, and [VO 4 ] in the quest for nonlinear optical materials1M 3 MoO 4 (HCO 3 ) (M = Rb and Cs): cation-tuned synthesis of two noncentrosymmetric molybdate-carbonates with isolated [MoO 4 ] and [HCO 3 ] groups0Na 2 PbB 6 O 10 SO 4 and Ca 2.58 Pb 0.42 B 6 O 11 SO 4 : first borate–sulfates featuring 3D porous borate anionic frameworks0层状结构深紫外非线性光学晶体研究进展（特邀）2新型非线性光学晶体和双折射晶体的研究进展（特邀）4混合阴离子无水无机硼酸盐深紫外非线性光学晶体的研究进展（特邀）4Size effect of cations in the A2B3O4F3 family: Based on the new member Cs2B3O4F34Engineering 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 Substitution6Review of KBe2BO3F2-like second-order nonlinear optical materials and their structure-performance relationships13Na[B3IO7(OH)] and Na2[B4IO9](IO3): Explorations of Boroiodates with Strong Second Harmonic Generation Response and Large Birefringence54(NH4)Na3Zn4(PO4)4:An open-framework zincophosphate exhibiting well-balanced optical and thermal performance1NH4B5O7(OH)2 and CsRbB10O14(OH)4·H2O: Two Hydroxyborates Feature Significant Optical Anisotropy and Contain 1∞[B5O7(OH)2] Chains1La(SO3NH2)2NO3·H2O: synergistic anion engineering of the first rare-earth nitrate sulfamate defying transparency-birefringence-nonlinearity trade-offs in ultraviolet nonlinear optics8Promising UV/DUV nonlinear optical materials with X-membered (X = multiples of 6) rings in anhydrous inorganic borates20Descriptors Assisted in Design High-performance Nonlinear Optical Materials with Donor-Acceptor Framework Systems0Variability of a Non‐Centrosymmetric Tecto‐Borosulfate: Introduction of Various Molecular Cations into BiX[B(SO 4 ) 2 ] 4 (X = H 3 O + , NO 2 + , NH 4 + , NO + )5Unlocking Advanced UV NLO Crystals in Rare‐Earth Metal Borate Fluorides via [B 3 O 6 ]‐Mediated Structural Modulation18Structural, spectral, dielectric, and nonlinear optical properties of 2,4,6-Trinitrophenol with optical limiting behavior3Mössbauer Spectroscopy on Antimony Borosulfates Reveals Weak Coordination Behavior1Mößbauer‐Spektroskopie an Antimon‐Borosulfaten belegt deren schwache Koordinationskraft1Chiral Eu–K Metal–organic Framework Based on Lactate Derivative and Its Second-Order Nonlinear Optical Properties0CsB(OH) 4 (H 2 O) 2 and Na(NH 4 ) 2 B 10 O 16 OH(H 2 O): a hydroxylation modification strategy regulates the borate structures and optical properties0[Sr(H 2 O)]{Sr[B(OH) 3 ]}[B 5 O 8 (OH)] 2 : A Deep-Ultraviolet Second-Order Nonlinear Optical Strontium Borate Constructed by Mixing π-Conjugated and Non-π-Conjugated Units1Ba 4 CdGa 2 S 6 F 4 : A Chalcohalide Birefringent Crystal with Large Band Gap Designed by the Cation and Anion Cosubstitution Strategy2Significant Enhancement of Birefringence Resulting from the Introduction of [BO 2 (OH)] Groups into Borosulfates0Topology-symmetry analysis and structure prediction in nonlinear optical AB4O6F (A = Na, K, Rb, Cs, NH4) and AAlB3O6F (A = K, Rb, Cs) polytypes1The Achievement of a Strong Second Harmonic Generation Response and a Large Birefringence in Sulfates4Topological structural chemistry of fluorooxoborates: From fundamental building blocks to macroscopic optical performance regulation0Toward the vacuum-ultraviolet frontier in nonlinear optical frequency conversion: phase-matching mechanisms across dimensions and architectures2Designing Novel Solar‐Blind Ultraviolet Nonlinear Optical Crystals Based on Local Proton Distribution Complementary Effect0Designing Novel Solar‐Blind Ultraviolet Nonlinear Optical Crystals Based on Local Proton Distribution Complementary Effect0Accelerating the Discovery of Deep-Ultraviolet Nonlinear Optical Materials by Combining Machine Learning Interatomic Potentials with First-Principles Calculations: A Case of LiB2O3F0Borophosphate-based second-order nonlinear optical materials: Advances in structural diversity and optical performance0

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  1. Dramatically improved optical anisotropy by realizing stereochemically active lone pairs in a sulfate system, K 2 SO 4 ·HIO 3

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  2. Enhancement of birefringence and refractive index dispersion optimization from iodates to fluorooxoiodates

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  3. K 5 [B 3 O 3 F 4 (OH)] 2 (NO 3 ): the first hydroxyfluorooxoborate-nitrate with a short ultraviolet cutoff edge and large birefringence

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  4. Linear π-conjugated units of the D ∞h point group as superior ultraviolet birefringent units

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  5. Mg 2 Pb 2 Si 2 O 7 F 2 : a new lead-containing alkali earth metal silicate fluoride with a short cutoff edge

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  6. Recent progress in borate-based short-wavelength nonlinear optical crystals with boron–oxygen skeleton modification

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  7. Synthesis and characterization of Cs 2 Zn 4 V 4 O 15 —a new vanadate in the Cs–Zn–V–O quaternary system

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  8. Synthesis, structures and properties of two new selenite optical materials: K 2 Zn 3 Se 4 O 12 and K 4 Zn 3 V 4 Se 2 O 19

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  9. BaB2P2O8F2: A Fluoroborophosphate with [B2P2O8F2]∞ Layers and Deep-Ultraviolet Cutoff Edge

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  10. Ba2B9O13F4·BF4: first fluorooxoborate with unprecedented infinite [B18O26F8] tubes and deep-ultraviolet cutoff edge

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  11. Recent Development of Sn II , Sb III ‐based Birefringent Material: Crystal Chemistry and Investigation of Birefringence

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  12. Recent Development of SnII, SbIII‐based Birefringent Material: Crystal Chemistry and Investigation of Birefringence

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  13. Na2BaB12O18F4: A Mixed Alkali/Alkaline-Earth Metal Fluorooxoborate with Two Unprecedented Interpenetrating Three-Dimensional B–O/F Anionic Networks and a Short Ultraviolet Cutoff Edge

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  14. Theoretical Prediction‐Assisted Synthesis and Characterization of Infrared Nonlinear Optical Material NaSrBS3

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  15. Cs 3 [(BOP) 2 (B 3 O 7 ) 3 ]: A Deep-Ultraviolet Nonlinear Optical Crystal Designed by Optimizing Matching of Cation and Anion Groups

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  16. Hg3(SeO3)2(SO4): A UV Nonlinear Optical Mercury Selenite Sulfate Constructed by Neat [Hg6O8(SeO3)4]∞ Layers and SO4 Tetrahedra

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  17. Target-Oriented Synthesis of Borate Derivatives Featuring Isolated [B3O3] Six-Membered Rings as Structural Features

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  18. Ultraviolet Crystal with Strong Optical Nonlinearity by Creating Halogen-Centered Secondary Building Blocks

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  19. A survey of stereoactive oxysalts for linear and nonlinear optical applications

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  20. Three Borates Belonging to the A(I)7Ae(II)Re(III)2B15O30 Family as Promising Nonlinear Optical Crystals

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  21. Binary Heterogroup-Templated Scaffolds of Polyoxopalladates as Precatalysts for Plasma-Assisted Ammonia Synthesis

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  23. Na 6 Mg 3 P 4 S 16 and RbMg 2 PS 4 Cl 2 : two Mg-based thiophosphates with ultrawide bandgaps resulting from [MgS 6 ] and [MgS x Cl 6− x ] octahedra

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  24. A2Hgx(SeO3)y (A = K, Rb, Cs): Three Alkali Metal Mercury Selenites Featuring Unique 1D [HgOm(SeO3)n]∞ Chains

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

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  26. Cd8(BO3)4SiO4: Metal Cation Inducing the Formation of Isolated [BO3] and [SiO4] Units in Borate Silicate

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  29. Exploration of antimony( iii ) oxyhalides via single-site substitution in quest of large birefringence

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  30. K, Rb-hydroxyborates series with deep-ultraviolet KRbB 5 O 8 (OH) possessing moderate second harmonic generation response

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  31. NaB(OH) 3 CH 3 : a deep-ultraviolet optical crystal with unprecedented methyl-modified [B(OH) 3 CH 3 ] units

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

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  33. Structural characterisation and optical properties of new alkaline earth phosphate CaMg(P 4 O 12 ) and alkaline alumophosphate Cs 3 Al 4 (PO 4 ) 5

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  34. 新型深紫外非线性光学晶体研究进展（特邀）

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  35. Toward the ultraviolet (UV) or deep-UV nonlinear optical crystals: The combination of π-conjugated planar [XY3] and tetrahedral [XY4]

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  36. AYSO4F2 (A = K, Rb): [YO4F4] Polyhedra Enhancement of Birefringence in Non-π-Conjugated Sulfate Systems

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  37. A perspective on deep-ultraviolet nonlinear optical materials

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

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  39. 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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  40. Structure‐Prediction‐Oriented Synthesis of Thiophosphates as Promising Infrared Nonlinear Optical Materials

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  41. Structure‐Prediction‐Oriented Synthesis of Thiophosphates as Promising Infrared Nonlinear Optical Materials

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  42. Enhanced UV Nonlinear Optical Properties in Layered Germanous Phosphites through Functional Group Sequential Construction

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  43. Enhanced UV Nonlinear Optical Properties in Layered Germanous Phosphites through Functional Group Sequential Construction

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  44. Fluorine-driven materials design of novel deep-ultraviolet nonlinear optical crystal materials: Research progress and challenges

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  45. A3Sc(SO4)3 (A = K, Rb, Cs): Three Deep‐Ultraviolet Transparent Alkali‐Scandium Sulfates with Strong Second‐Harmonic Generation Response and High Thermal Stability

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  46. NH4Y(SO4)2·H2O and NH4YSO4F2: Two New Ammonium‐Rare Earth Metal Sulfates with Enhanced Optical Anisotropy and Deep Ultraviolet Transmission

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  47. Tunable Intracavity Coherent Up‐Conversion with Giant Nonlinearity in a Polar Fluidic Medium

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  48. The Directional Design of the Quasi‐Phase‐Matching Short‐Wave Ultraviolet Nonlinear Optical Crystal

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  49. Sulfate Derivatives with Heteroleptic Tetrahedra: New Deep‐Ultraviolet Birefringent Materials in which Weak Interactions Modulate Functional Module Ordering

    Angewandte Chemie International Edition · 2024-08-15

    Huan Zhou, Meng Cheng, Dongdong Chu, Xu Liu, Ran An, Shilie Pan, Shilie Pan, Zhihua Yang

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  50. Sulfate Derivatives with Heteroleptic Tetrahedra: New Deep‐Ultraviolet Birefringent Materials in which Weak Interactions Modulate Functional Module Ordering

    Angewandte Chemie · 2024-08-15

    Huan Zhou, Meng Cheng, Dongdong Chu, Xu Liu, Ran An, Shilie Pan, Zhihua Yang

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