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RESEARCH PAPER · National Science Review · 2022

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

Bingliang Cheng, Zi‐Jian Li, Yu Chu, Abudukadi Tudi, Miriding Mutailipu, Fangfang Zhang, Zhihua Yang, Shilie Pan

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(NH4)3B11PO19F3: a deep-UV nonlinear optical crystal with unique [B5PO10F]∞ layersOriginalA 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 birefringence17Large 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 edge8Difluoro(oxalato)borates as Short-Wavelength Optical Crystals with Bifunctional [BF 2 C 2 O 4 ] Units38NaB3O4F(OH): A Hydroxyfluorooxoborate with One-Dimensional Chain Featuring Large Birefringence and Short Ultraviolet Cutoff Edge5The Microscopic Origin of Second Harmonic Generation Response: The Spatial Structure of Instantaneous Dipole Moments in Electron Excitation8The Microscopic Origin of Second Harmonic Generation Response: The Spatial Structure of Instantaneous Dipole Moments in Electron Excitation1NaK5Zn2(B5O10)2 and β-K3ZnB5O10: Two Zincoborates with Deep-UV Cutoff Edge9Sn3B10O17Cl2 Achieving Birefringence Enhancement by Stereochemical Activity Lone Pair9Li2PbB2O5: 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 Template95Li0.5Na0.5AlB2O4F2: Fluoroaluminoborate with Aligned 1∞[BO2] Chain Induced by Unprecedented [AlO3F3]6− Species Features Enhanced Birefringence30LiNaB6O9F2: A Promising UV NLO Crystal Having Fluorine‐Directed Optimal Performances and Double Interpenetrating 3[B6O9F2]∞ Networks33Rb 3 B 5 O 8 F 2 and K 0.6 Rb 2.4 B 5 O 8 F 2 : two new deep-ultraviolet transparent nonlinear optical fluorooxoborates designed by cation regulation13Design of deep-ultraviolet nonlinear optical materials based on fundamental building blocks with excellent microscopic properties1Enhancement of birefringence and refractive index dispersion optimization from iodates to fluorooxoiodates1Enhancing birefringence of non-π-conjugated sulfate systems through rare-earth metal-centered polyhedra10Evaluating refractive index and birefringence of nonlinear optical crystals: Classical methods and new developments45K 5 [B 3 O 3 F 4 (OH)] 2 (NO 3 ): the first hydroxyfluorooxoborate-nitrate with a short ultraviolet cutoff edge and large birefringence18LiCs 3 AlB 7 O 14 : achieving enhanced optical anisotropy via [AlO 4 ] tetrahedron introduction to rearrange the anionic framework5Linear π-conjugated units of the D ∞h point group as superior ultraviolet birefringent units1MB 3 P 2 S 10 (M = Rb, Cs): two new alkali metal thioboratephosphates with [B 6 P 4 S 20 ] T3-supertetrahedra2Mg 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 system5Tetrahedron-based deep-ultraviolet nonlinear optical crystal with optimized KBe 2 BO 3 F 2 -like structure and disordered cations2BaB2P2O8F2: A Fluoroborophosphate with [B2P2O8F2]∞ Layers and Deep-Ultraviolet Cutoff Edge4Rational 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 System15Structure and Characterization of K2Na3B2P3O13, a New Nonlinear Optical Borophosphate with One-Dimensional Chain Structure and Short Ultraviolet Cutoff Edge13Controlling the Nonlinear Optical Behavior and Structural Transformation with A‐Site Cation in α‐AZnPO4 (A = Li, K)20Recent advances of inorganic phosphates with UV/DUV cutoff edge and large second harmonic response7Ba2B9O13F4·BF4: first fluorooxoborate with unprecedented infinite [B18O26F8] tubes and deep-ultraviolet cutoff edge14Na2BaB12O18F4: 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 NaSrBS324“Cation Activation”: An Effective Strategy for the Enhancement of Birefringence36Design of the Ionic Organic Nonlinear Optical Material NH 4 [LiC 3 H(CH 3 )O 4 ] with Ultrawide Band Gap and Moderate Birefringence79Design of the Ionic Organic Nonlinear Optical Material NH 4 [LiC 3 H(CH 3 )O 4 ] with Ultrawide Band Gap and Moderate Birefringence9Cs 3 [(BOP) 2 (B 3 O 7 ) 3 ]: A Deep-Ultraviolet Nonlinear Optical Crystal Designed by Optimizing Matching of Cation and Anion Groups169Target-Oriented Synthesis of Borate Derivatives Featuring Isolated [B3O3] Six-Membered Rings as Structural Features20Three Polyborates with High-Symmetry [B12O24] Units Featuring Different Dimensions of Anion Groups8From Monofluorophosphates A2PO3F to Difluorophosphates APO2F2 (A = alkali metal): Design of a Potential Deep-Ultraviolet Nonlinear Optical Materials System with a Shortened Phase-Matching Wavelength41Ultraviolet Crystal with Strong Optical Nonlinearity by Creating Halogen-Centered Secondary Building Blocks15Fluorooxoborate Promoting the Exploration of Short-Wavelength Linear and Nonlinear Optical Crystals with Expected Properties and Versatile Structures27The Strategy to Improve the Phase Matching Ability in Tetrahedron‐Based Deep‐Ultraviolet Nonlinear Optical Crystals21Introduction of the [B–O/F] Units Enhances the Band Gap and Birefringence from Na6Mg3B10O18F6 to K3NaB10O16F211Three Borates Belonging to the A(I)7Ae(II)Re(III)2B15O30 Family as Promising Nonlinear Optical Crystals12A methodical investigation on the growth and characterization of a third-order nonlinear optical novel co-crystal of 8-hydroxyquinolinium phthalate: X-ray, Hirshfeld surface, optical, mechanical, thermal and DFT analysis13Sr(NO 3 )(NH 2 SO 3 )·H 2 O: First Nitrate Sulfamate Revealing Remarkable Second Harmonic Generation and Optimized Birefringence25YSO4F·H2O: A Deep-Ultraviolet Birefringent Rare-Earth Sulfate Fluoride with Enhanced Birefringence Induced by Fluorinated Y-Centered Polyhedra19Ba 4 B 14 O 25 : A Deep Ultraviolet Transparent Nonlinear Optical Crystal with Strong Second Harmonic Generation Response Achieved by a Boron‐Rich Closed‐Loop Strategy12Deep‐Ultraviolet Transparent Mixed Metal Sulfamates with Enhanced Nonlinear Optical Properties and Birefringence11Deep‐Ultraviolet Transparent Mixed Metal Sulfamates with Enhanced Nonlinear Optical Properties and Birefringence75PbTeB 4 O 9 : a lead tellurium borate with unprecedented fundamental building block [B 4 O 10 ] and large birefringence12Na 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 ] octahedra4A 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 Transmission10C(NH2)3Cd(C2O4)Cl(H2O)·H2O and BaCd(C2O4)1.5Cl(H2O)2: Two Oxalate Chlorides Obtained by Chemical Scissors Strategy Exhibiting Low-Dimensional Structural Networks and Balanced Overall Optical Properties14Cd8(BO3)4SiO4: Metal Cation Inducing the Formation of Isolated [BO3] and [SiO4] Units in Borate Silicate15Fluorination strategy toward chemical and functional modification65“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 birefringence10Exploring short-wavelength birefringent crystals via triggering cooperative arrangement between different π-conjugated groups8K 2 MgMoP 2 O 10 and K 3 Mg 2 MoP 3 O 14 : two new molybdophosphates exhibiting different optical anisotropies induced by variable dimensionality of the anion framework4K, 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 ) 51Syntheses, structures and characterization of noncentrosymmetric MZnPO 4 (M = K, NH 4 )4新型深紫外非线性光学晶体研究进展（特邀）9Hierarchical van der Waals Assemblies to Boost Deep‐Ultraviolet Nonlinear‐Optical Capabilities in Boron Phosphate8Screening Large Birefringent Materials via Halogen Regulation in Ternary d0-Transition Metal Oxyhalides8Dual-Anion Strategy Induces Dual Enhancement Toward Ultrashort Phase-Matching Wavelength in Deep-UV Transparent d0 Transition Metal Oxyfluorides21KPO2(NHCONH2)2: A Promising Deep-Ultraviolet Nonlinear Optical Phosphate Containing Polar [PO2(NHCONH2)2]− Tetrahedra15Trithionic guanidine: A novel semi-organic short-wave ultraviolet nonlinear optical sulfate with dimeric heteroleptic tetrahedra14Unleashing the potential of π-conjugated [B2O3(OH)2] to enhance birefringence in DUV crystals9Extending Unique 1D Double-Chains to 2D Layers with Birefringent Gain by Introducing a Hydroxyl Group5A 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 Edges6Na3[Al2B6P4O22(OH)3](H2O)6 and Na3[Al2BP2O11](H2O)0.5: Two Remarkable Complex Aluminum Borophosphates82D Materials‐Based Pulsed Solid‐State Laser: Status and Prospect18Structure‐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 challenges6Na2B6SO13 with unprecedented [B6SO13]∞ double chains and largest birefringence among borosulfates induced by the uniform arrangement of [B3O7] units19Achieving the Birefringence Optimization by Methyl Modulation in Organic Nonlinear Optical Crystals15A2Cd(PO3)4 (A = K, Rb, Cs): Series of cadmium polyphosphates with infinite 1[(PO3)4]ꝏ chains and deep ultraviolet transparency windows2Li2NaB3S2O12: A Deep-UV Transparent Borosulfate with Moderate Birefringence Derived from the [B3S2O12]∞ Infinite Chain Designed by the High Boron-to-Sulfur Ratio Strategy6Amino substitution strategy achieves significant blue shift while preserving high optical anisotropy: A2(H3C3N4S2)2•H2O (A =NH4, K, Rb, Cs)6Rb 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)12Designing a Heteroleptic Tetrahedral Group with an Ultrahigh Polarizability Anisotropy by Optimizing the Bonding Electrons Activity and Their Distribution14Li3[AlP2O7F(OH)](H2O)0.5 and A[Al2(PO4)2F(H2O)](A = K, Rb): Counter Cation Templates Derived Three Polar Alkaline Metal Fluoroaluminophosphates6Deep 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 Performances17Anion ratio-directed design of CaB 4 O 5 F 4 and CaB 6 O 8 F 4 : [BO 3 ]/[BO 2 F 2 ] hybridization tailoring deep-ultraviolet nonlinear optical performance2BaAlPO 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 edge3Hg 2 (HTe 2 O 5 )(PO 4 ): a novel phosphate crystal with enhanced birefringence enabled by the synergistic modification of multiple functional groups12Li 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 2 Al 2 Ti(PO 4 ) 4 (M = Rb, Cs): synthesis and optical property investigation of two titanium phosphates with a dissimilar structural configuration2M 3 MoO 4 (HCO 3 ) (M = Rb and Cs): cation-tuned synthesis of two noncentrosymmetric molybdate-carbonates with isolated [MoO 4 ] and [HCO 3 ] groups0Optimizing optical anisotropy in low-dimensional structures via intralayer hydrogen bonding modulation and anionic substitution17RbB 7 O 10 (OH) 2 and NaB 11 O 16 (OH) 2 : alkali metal hydroxyborates with two-dimensional layered structures and large birefringence1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）4Birefringence Modulation by Phenyl and Acyl Groups in Urea-Based Crystals3Na3Y2F3P2O8 and K4Y3F5P4O14: [YOF] Polyhedra Inducing Birefringence Enhancement in Non-π-Conjugated Phosphate Systems3Size effect of cations in the A2B3O4F3 family: Based on the new member Cs2B3O4F34Three Cases of Borates with Different Dimensional Frameworks Induced by Metal Cations1A Promising Deep Ultraviolet Nonlinear Optical Crystal Activated by the Ordered Structure Design40A Promising Deep Ultraviolet Nonlinear Optical Crystal Activated by the Ordered Structure Design3Rb 7 PbY 2 (B 5 O 10 ) 3 : A Noncentrosymmetric Rare-Earth Borate Nonlinear Optical Crystal with [B 5 O 10 ] Unit16Metal Cation Engineered UV Birefringent Crystals in π‐Conjugated Sulfonates with Record‐High Optical Anisotropy17[CON3H6BF4]: An Efficient Metal‐Free Borate with Optimized Birefringence Achieved by Structural Design Strategy15Syntheses, structural characterization, and nonlinear optical properties of mixed alkaline/alkaline earth metal borophosphates1Anion-Ordered [B3O5(OH)2] Induced by Crystal Water with Deep Ultraviolet Transparency and Large Birefringence in Boron-Rich Borophosphates4Ag(Te2O3)(PO4): The first Ag-containing phosphate-tellurite nonlinear optical crystal featuring novel zigzag layered structure0Growth and Characterization of Novel SrB2O4 Crystals0Dual-anion synergy drives remarkable birefringence in sulfate–nitrate crystals1K 6 Mo 8 PO 29 OH·H 2 O and K 6 Mo 5 P 2 O 23 ·7H 2 O: strongly distorted [MoO 6 ] octahedral groups effectively enhance birefringence0CsB(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 properties0K 7 MgY 2 (B 5 O 10 ) 3 : a novel ultraviolet nonlinear optical crystal based on the [B 5 O 10 ] functional unit2Realization of the transition from an indirect band gap to a direct band gap through halogen regulation in the Cs–Ag–X system1Regulating KBBF-like structures via a charge-assisted hydrogen-bonded framework to enable easily grown ultraviolet nonlinear optical crystals0孤对电子效应羟基硼酸盐非线性光学研究进展（特邀）0Constructing Deep‐Ultraviolet Nonlinear Optical Crystals via Synergistic Combination of Fluorinated Polyhedra and Polymerized BO 3 Units15Topology-symmetry analysis and structure prediction in nonlinear optical AB4O6F (A = Na, K, Rb, Cs, NH4) and AAlB3O6F (A = K, Rb, Cs) polytypes1Magnesium Methylphosphonate Ultraviolet Nonlinear Optical Crystal With Ultrawide Bandgap and Strong Second‐Harmonic Generation Response0Cs4Ag9I12Cl: A congruent-melting semiconductor crystal with a photoluminescence fast decay component of 3.3 ns by halogen regulation0Interpretable Machine Learning for Bandgap Prediction and Descriptor‐Guided Design Rules of Phosphates1Regulating B‐O Arrangement Boosts Anisotropy in a Simple Rubidium Borate, Leading to a High‐Performance UV NLO Crystal0Design of deep-ultraviolet nonlinear optical BePNO2 guided by non-π-conjugated NLO-active unit0Toward the vacuum-ultraviolet frontier in nonlinear optical frequency conversion: phase-matching mechanisms across dimensions and architectures2Computational prediction of promising deep-UV nonlinear optical borate fluorides SrBO2F and BaBO2F0A Rare-Earth Borophosphate Ultraviolet Nonlinear Optical Crystal Featuring P–O–P Linkages0Accelerating the Discovery of Deep-Ultraviolet Nonlinear Optical Materials by Combining Machine Learning Interatomic Potentials with First-Principles Calculations: A Case of LiB2O3F0

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

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

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  36. “Cation Activation”: An Effective Strategy for the Enhancement of Birefringence

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  37. Design of the Ionic Organic Nonlinear Optical Material NH 4 [LiC 3 H(CH 3 )O 4 ] with Ultrawide Band Gap and Moderate Birefringence

    Angewandte Chemie International Edition · 2023-05-22

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  38. Design of the Ionic Organic Nonlinear Optical Material NH 4 [LiC 3 H(CH 3 )O 4 ] with Ultrawide Band Gap and Moderate Birefringence

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

    Journal of the American Chemical Society · 2023-05-26

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

    Inorganic Chemistry · 2023-05-31

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  41. Three Polyborates with High-Symmetry [B12O24] Units Featuring Different Dimensions of Anion Groups

    ACS Omega · 2023-06-02

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  42. From Monofluorophosphates A2PO3F to Difluorophosphates APO2F2 (A = alkali metal): Design of a Potential Deep-Ultraviolet Nonlinear Optical Materials System with a Shortened Phase-Matching Wavelength

    Chemistry of Materials · 2023-07-06

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

    Chemistry of Materials · 2023-07-06

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  44. Fluorooxoborate Promoting the Exploration of Short-Wavelength Linear and Nonlinear Optical Crystals with Expected Properties and Versatile Structures

    Chemistry of Materials · 2023-07-07

    Bingliang Cheng, Wenjuan Ma, Abudukadi Tudi, Fangfang Zhang, Zilong Chen, Xueling Hou, Zhihua Yang, Shilie Pan

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

    Advanced Optical Materials · 2023-07-09

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  46. Introduction of the [B–O/F] Units Enhances the Band Gap and Birefringence from Na6Mg3B10O18F6 to K3NaB10O16F2

    Inorganic Chemistry · 2023-07-26

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

    Crystal Growth & Design · 2023-08-21

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  48. A methodical investigation on the growth and characterization of a third-order nonlinear optical novel co-crystal of 8-hydroxyquinolinium phthalate: X-ray, Hirshfeld surface, optical, mechanical, thermal and DFT analysis

    Materials Research Bulletin · 2023-09-03

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  49. 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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  50. YSO4F·H2O: A Deep-Ultraviolet Birefringent Rare-Earth Sulfate Fluoride with Enhanced Birefringence Induced by Fluorinated Y-Centered Polyhedra

    Inorganic Chemistry · 2023-10-12

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