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RESEARCH PAPER · Angewandte Chemie International Edition · 2021

Achieving Short‐Wavelength Phase‐Matching Second Harmonic Generation in Boron‐Rich Borosulfate with Planar [BO3] Units

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

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Achieving Short‐Wavelength Phase‐Matching Second Harmonic Generation in Boron‐Rich Borosulfate with Planar [BO3] UnitsOriginalAZn 2 (BO 3 )Si 2 O 5 (A = Rb, Cs): first examples of KBe 2 BO 3 F 2 structure type in the borosilicate family exhibiting a deep-ultraviolet cutoff edge25A 2 B 6 O 9 F 2 (A = NH 4 , K): new members of A 2 B 6 O 9 F 2 family with deep-UV cutoff edges and moderate birefringence17BaI 3 O 9 H: a new alkaline-earth metal hydroxy iodate with two groups2Large optical anisotropy-oriented construction of a carbonate-nitrate chloride compound as a potential ultraviolet birefringent material44Li 7 SrScB 12 O 24 and Li 7 Ba 0.6 Ca 0.4 ScB 12 O 24 : two new quaternary rare-earth borates with short UV cutoff edges4Na 3 YB 8 O 15 : a new rare-earth borate with an infinite one-dimensional [B 8 O 15 ] ∞ chain and a short ultraviolet cutoff edge8Finding the First Squarates Nonlinear Optical Crystal NaHC4O4·H2O with Strong Second Harmonic Generation and Giant Birefringence56Promising Deep‐Ultraviolet Birefringent Materials via Rational Design and Assembly of Planar π‐Conjugated [B(OH)3] and [B3O3(OH)3] Functional Species6Promising Deep‐Ultraviolet Birefringent Materials via Rational Design and Assembly of Planar π‐Conjugated [B(OH)3] and [B3O3(OH)3] Functional Species83Second-Harmonic Generation-Positive Na 2 Ga 2 SiS 6 with a Broad Band Gap and a High Laser Damage Threshold14(NH4)3B11PO19F3: a deep-UV nonlinear optical crystal with unique [B5PO10F]∞ layers142Difluoro(oxalato)borates as Short-Wavelength Optical Crystals with Bifunctional [BF 2 C 2 O 4 ] Units38The Unconventional Cadmium Borosulfates Cd[B2O(SO4)3] and Cd4[B2O(SO4)6]4NaK5Zn2(B5O10)2 and β-K3ZnB5O10: Two Zincoborates with Deep-UV Cutoff Edge9Li2PbB2O5: A Pyroborate with Large Birefringence Induced by the Synergistic Effect of Stereochemical Active Lone Pair Cations and π-Conjugated [B2O5] Groups14Exploring Short-Wavelength Phase-Matching Nonlinear Optical Crystals by Employing KBe2BO3F2 as the Template95LiNaB6O9F2: A Promising UV NLO Crystal Having Fluorine‐Directed Optimal Performances and Double Interpenetrating 3[B6O9F2]∞ Networks33KREP2Se6 (RE = Sm, Gd, Tb): The First Rare‐Earth Selenophosphates with Remarkable Nonlinear Optical Activities Realized by Synergistic Effect of RE‐ and P‐Based Motifs39Rb 3 B 11 P 2 O 23 : Materials Design of a New Chemically Benign Deep-Ultraviolet Nonlinear Optical Material58A lithium–scandium sulfate with second-harmonic generation response and deep-ultraviolet transparency7Enhancement of birefringence and refractive index dispersion optimization from iodates to fluorooxoiodates1Enhancing birefringence of non-π-conjugated sulfate systems through rare-earth metal-centered polyhedra10K 5 [B 3 O 3 F 4 (OH)] 2 (NO 3 ): the first hydroxyfluorooxoborate-nitrate with a short ultraviolet cutoff edge and large birefringence18KNa 2 La 2 (BO 3 ) 3 : a shortite-type lanthanide borate exhibiting strong nonlinear optical activity induced by isolated [BO 3 ] triangles and distorted [LaO 9 ] polyhedra26Linear 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 192Tetrahedron-based deep-ultraviolet nonlinear optical crystal with optimized KBe 2 BO 3 F 2 -like structure and disordered cations2Two UV optical crystals with strong optical anisotropy, large band gaps and an α-BBO type structure7Rational Design of the First Ammonium Magnesium Borate with Deep-Ultraviolet Cutoff Edge and Moderate Birefringence and Further Investigation into the Nature of Ammonium in the Borate System15Ba2B9O13F4·BF4: first fluorooxoborate with unprecedented infinite [B18O26F8] tubes and deep-ultraviolet cutoff edge14Chain‐like [S x ] ( x =2–6) Units Realizing Giant Birefringence with Transparency in the Near‐Infrared for Optoelectronic Materials53Chain‐like [S x ] ( x =2–6) Units Realizing Giant Birefringence with Transparency in the Near‐Infrared for Optoelectronic Materials5Theoretical Prediction‐Assisted Synthesis and Characterization of Infrared Nonlinear Optical Material NaSrBS324AAl(Te 4 O 10 ) (A = Na, Ag) and K 2 Ga 2 (HTe 6 O 16 )(HTeO 3 ): Three Aluminum/Gallium Tellurites with Large Birefringence and Wide Band Gap21The Strategy to Improve the Phase Matching Ability in Tetrahedron‐Based Deep‐Ultraviolet Nonlinear Optical Crystals21Nonlinear optical inorganic sulfates: The improvement of the phase matching ability driven by the structural modulation41Three Borates Belonging to the A(I)7Ae(II)Re(III)2B15O30 Family as Promising Nonlinear Optical Crystals12Sr(NO 3 )(NH 2 SO 3 )·H 2 O: First Nitrate Sulfamate Revealing Remarkable Second Harmonic Generation and Optimized Birefringence25Ultrashort Phase‐Matching Wavelength and Strong Second‐Harmonic Generation in Deep‐UV‐Transparent Oxyfluorides by Covalency Reduction33Ultrashort Phase‐Matching Wavelength and Strong Second‐Harmonic Generation in Deep‐UV‐Transparent Oxyfluorides by Covalency Reduction3Na 10 Zn(NO 3 ) 4 (SO 3 S) 4 : a nonlinear optical crystal combining inorganic π-conjugated and non-π-conjugated heteroanion groups8A Sharp Improvement of Sulfate's Birefringence Induced by the Synergistic Effect of Heteroleptic and Dimeric Strategies14K 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 tetrahedra8A UV non-hydrogen pure selenite nonlinear optical material for achieving balanced properties through framework-optimized structural transformation41CsAlB 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] tetrahedra5K, 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 templates153Synthesis and Characterization of Metal Iso-cyamelurate K0.5In0.5(H2C6N7O3)2·9H2O with Large Birefringence8The Birefringence Modulation in Short‐Wave Ultraviolet Sulfates with Functional π‐Conjugated Cations and Polymerized Heteroleptic Tetrahedral Anions18Enhanced 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 Construction116NH4Y(SO4)2·H2O and NH4YSO4F2: Two New Ammonium‐Rare Earth Metal Sulfates with Enhanced Optical Anisotropy and Deep Ultraviolet Transmission3Sulfate 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 Ordering4Na2B6SO13 with unprecedented [B6SO13]∞ double chains and largest birefringence among borosulfates induced by the uniform arrangement of [B3O7] units19Li2NaB3S2O12: A Deep-UV Transparent Borosulfate with Moderate Birefringence Derived from the [B3S2O12]∞ Infinite Chain Designed by the High Boron-to-Sulfur Ratio Strategy6The design of a non-centrosymmetric structure in sulfates by cation-induced symmetry breaking4Rb 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)12Unveiling Charge Dependent Law to Enhance Birefringence in 2‐Aminopyrimidine Family21Deep ultraviolet transparent borophosphates LiAB 2 P 2 O 9 (A = NH 4 , K) and LiNaB 2 P 2 O 8 (OH) 2 ·H 2 O exhibiting a moderate second-harmonic generation response4Emergent Mid‐Infrared Nonlinear Optical Candidates With Targeted Balance Performances17A strongly birefringent sulfate crystal with a wide second-harmonic generation phase-matching range4CsBO(OH) 2 : a new hydroxyborate with the rare [BO(OH) 2 ] group and a deep ultraviolet cutoff edge3K 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 birefringence2Li 2 CeRbB 18 O 30 and Li 2 Cs 2 SrB 18 O 30 : promising low-birefringence materials for UV and deep UV zero-order waveplates4M 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 frameworks0Stereochemically active lone pair-induced large optical anisotropy in a novel infrared birefringent crystal Ba 2 La 2 Sb 4 S 10 (S 2 )5Structure modulation by cationic modification of sulfates using planar CS(NH 2 ) 25Y(C 6 H 5 SO 3 ) 3 ·9H 2 O: strategic integration of ligand substitution and π-conjugated group linkage in sulfates for enhanced ultraviolet nonlinear optical properties4新型非线性光学晶体和双折射晶体的研究进展（特邀）4Highly Polarizable Phosphorus‐Centered Tetrahedra and π‐Conjugated Carbon‐Centered Triangular Moieties Inducing Large Anisotropy and Short‐Wavelength Phase‐Matching23Lithium Borate-Squarate: An Organic–Inorganic Groups-Mixed Nonlinear Optical Crystal with Large Birefringence4Polar [ NH ( CH2SO3 )2]2− Dimers Enable the First Promising Iminodimethanesulfonate with Nonlinear Optical Properties and Wide UV Transparency19Metal Cation Engineered UV Birefringent Crystals in π‐Conjugated Sulfonates with Record‐High Optical Anisotropy17Synthesis and Characterization of (H7C5N2)6(V10O28)·2H2O with Edge-Sharing VO6 Octahedra Exhibiting Large Birefringence2Giant Birefringence and Strong Third-Order Nonlinear Optical Response in a Hybrid Crystal Templated by a Push–Pull π-Conjugated System6La(SO3NH2)2NO3·H2O: synergistic anion engineering of the first rare-earth nitrate sulfamate defying transparency-birefringence-nonlinearity trade-offs in ultraviolet nonlinear optics8Variability 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 + )5Synthesis and Crystal Structure of Rb[B(SO 4 ) 2 ]: A Borosulfate Obtained from a Reaction with Chlorosulfuric Acid0Two-dimensional graphene-like BeO sheet: a promising deep-ultraviolet nonlinear optical material with strong and highly tunable second harmonic generation5Dual-anion synergy drives remarkable birefringence in sulfate–nitrate crystals1Chiral calcium thiocyanate hybrids: amino acid-enabled structural diversity and second-harmonic generation0Synergism of [C 2 N 4 H 7 S] cations and anionic modulators: tailoring second-order nonlinear optics and birefringence in organic–inorganic crystals6(NH 4 )[B 4 O 5 (PO 4 )] – A Boron Rich Three-Dimensional Borophosphate1Ba 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 Borosulfates0The Achievement of a Strong Second Harmonic Generation Response and a Large Birefringence in Sulfates4An Ultraviolet Transparent Nonlinear Optical Crystal Assembled from a Polarizable Tetrahedral Unit1NaNO 3 [(NH 2 ) 2 SO 2 ] 2 : A Halogen‐Free KBBF‐Type Nitrate Crystal with Record Birefringence for Ultraviolet Applications0Enhancing Birefringence of Sulphates by Polarity Modification in Planar Cations0Parallel arrangement of functional building blocks: toward performance synergy in oxalate borate ultraviolet nonlinear optical crystals0Two Rare Earth-Based Sulfates with Enhanced Birefringence and Broad Optical Transparency Window0A Hydrogen-Bonded Molecular Crystal with Strong Optical Anisotropy and Large Second-Harmonic Generation Response0Ratiometric Luminescent Thermo‐Hygrometry, Metal‐Dependent Second Harmonic Generation, and Humidity‐Variable Magnetic Relaxation in a Manganese(II)‐Doped Zinc(II) Molecular Halide0

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  1. AZn 2 (BO 3 )Si 2 O 5 (A = Rb, Cs): first examples of KBe 2 BO 3 F 2 structure type in the borosilicate family exhibiting a deep-ultraviolet cutoff edge

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  2. A 2 B 6 O 9 F 2 (A = NH 4 , K): new members of A 2 B 6 O 9 F 2 family with deep-UV cutoff edges and moderate birefringence

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  3. BaI 3 O 9 H: a new alkaline-earth metal hydroxy iodate with two groups

    New Journal of Chemistry · 2022-01-01

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  4. Large optical anisotropy-oriented construction of a carbonate-nitrate chloride compound as a potential ultraviolet birefringent material

    Chemical Science · 2022-01-01

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  5. Li 7 SrScB 12 O 24 and Li 7 Ba 0.6 Ca 0.4 ScB 12 O 24 : two new quaternary rare-earth borates with short UV cutoff edges

    New Journal of Chemistry · 2022-01-01

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  6. Na 3 YB 8 O 15 : a new rare-earth borate with an infinite one-dimensional [B 8 O 15 ] ∞ chain and a short ultraviolet cutoff edge

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

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  8. Promising Deep‐Ultraviolet Birefringent Materials via Rational Design and Assembly of Planar π‐Conjugated [B(OH)3] and [B3O3(OH)3] Functional Species

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  9. Promising Deep‐Ultraviolet Birefringent Materials via Rational Design and Assembly of Planar π‐Conjugated [B(OH)3] and [B3O3(OH)3] Functional Species

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  10. Second-Harmonic Generation-Positive Na 2 Ga 2 SiS 6 with a Broad Band Gap and a High Laser Damage Threshold

    Inorganic Chemistry · 2022-05-05

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  11. (NH4)3B11PO19F3: a deep-UV nonlinear optical crystal with unique [B5PO10F]∞ layers

    National Science Review · 2022-06-10

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  12. Difluoro(oxalato)borates as Short-Wavelength Optical Crystals with Bifunctional [BF 2 C 2 O 4 ] Units

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  13. The Unconventional Cadmium Borosulfates Cd[B2O(SO4)3] and Cd4[B2O(SO4)6]

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  14. NaK5Zn2(B5O10)2 and β-K3ZnB5O10: Two Zincoborates with Deep-UV Cutoff Edge

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  15. Li2PbB2O5: A Pyroborate with Large Birefringence Induced by the Synergistic Effect of Stereochemical Active Lone Pair Cations and π-Conjugated [B2O5] Groups

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

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  17. LiNaB6O9F2: A Promising UV NLO Crystal Having Fluorine‐Directed Optimal Performances and Double Interpenetrating 3[B6O9F2]∞ Networks

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  18. KREP2Se6 (RE = Sm, Gd, Tb): The First Rare‐Earth Selenophosphates with Remarkable Nonlinear Optical Activities Realized by Synergistic Effect of RE‐ and P‐Based Motifs

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

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  20. A lithium–scandium sulfate with second-harmonic generation response and deep-ultraviolet transparency

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

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  22. Enhancing birefringence of non-π-conjugated sulfate systems through rare-earth metal-centered polyhedra

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  23. 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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  24. KNa 2 La 2 (BO 3 ) 3 : a shortite-type lanthanide borate exhibiting strong nonlinear optical activity induced by isolated [BO 3 ] triangles and distorted [LaO 9 ] polyhedra

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

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

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  28. 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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  29. 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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  30. Tetrahedron-based deep-ultraviolet nonlinear optical crystal with optimized KBe 2 BO 3 F 2 -like structure and disordered cations

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  31. Two UV optical crystals with strong optical anisotropy, large band gaps and an α-BBO type structure

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  32. Rational Design of the First Ammonium Magnesium Borate with Deep-Ultraviolet Cutoff Edge and Moderate Birefringence and Further Investigation into the Nature of Ammonium in the Borate System

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

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  34. Chain‐like [S x ] ( x =2–6) Units Realizing Giant Birefringence with Transparency in the Near‐Infrared for Optoelectronic Materials

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  35. Chain‐like [S x ] ( x =2–6) Units Realizing Giant Birefringence with Transparency in the Near‐Infrared for Optoelectronic Materials

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

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    Yihan Yun, Mengfan Wu, Congwei Xie, Zhihua Yang, Guangmao Li, Shilie Pan

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  37. AAl(Te 4 O 10 ) (A = Na, Ag) and K 2 Ga 2 (HTe 6 O 16 )(HTeO 3 ): Three Aluminum/Gallium Tellurites with Large Birefringence and Wide Band Gap

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  38. The Strategy to Improve the Phase Matching Ability in Tetrahedron‐Based Deep‐Ultraviolet Nonlinear Optical Crystals

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    Hongyuan Sha, Yanran Shang, Zujian Wang, Rongbing Su, Chao He, Xiaoming Yang, Xifa Long

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  39. Nonlinear optical inorganic sulfates: The improvement of the phase matching ability driven by the structural modulation

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

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  41. Sr(NO 3 )(NH 2 SO 3 )·H 2 O: First Nitrate Sulfamate Revealing Remarkable Second Harmonic Generation and Optimized Birefringence

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  42. Ultrashort Phase‐Matching Wavelength and Strong Second‐Harmonic Generation in Deep‐UV‐Transparent Oxyfluorides by Covalency Reduction

    Angewandte Chemie International Edition · 2023-11-06

    Yilei Hu, Chao Wu, Xingxing Jiang, Kaining Duanmu, Zhipeng Huang, Zheshuai Lin, Mark Graeme Humphrey, Chi Zhang

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  43. Ultrashort Phase‐Matching Wavelength and Strong Second‐Harmonic Generation in Deep‐UV‐Transparent Oxyfluorides by Covalency Reduction

    Angewandte Chemie · 2023-11-06

    Yilei Hu, Chao Wu, Xingxing Jiang, Kaining Duanmu, Zhipeng Huang, Zheshuai Lin, Mark Graeme Humphrey, Chi Zhang

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  44. Na 10 Zn(NO 3 ) 4 (SO 3 S) 4 : a nonlinear optical crystal combining inorganic π-conjugated and non-π-conjugated heteroanion groups

    Inorganic Chemistry Frontiers · 2023-11-07

    Zihao Yu, Qingran Ding, Yuhang Jiang, Weiqi Huang, Changsheng Yang, Sangen Zhao, Junhua Luo

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  45. A Sharp Improvement of Sulfate's Birefringence Induced by the Synergistic Effect of Heteroleptic and Dimeric Strategies

    Small · 2023-12-10

    Hongyuan Sha, Yanran Shang, Zujian Wang, Rongbing Su, Chao He, Xiaoming Yang, Xifa Long

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

    Inorganic Chemistry · 2023-12-15

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