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RESEARCH PAPER · Chemistry of Materials · 2020

A 3 BBi(P 2 O 7 ) 2 (A = Rb, Cs; B = Pb, Ba): Isovalent Cation Substitution to Sustain Large Second-Harmonic Generation Responses

Lu Qi, Zhaohui Chen, Xuerui Shi, Xiaodong Zhang, Qun Jing, Na Li, Zhongqi Jiang, Bingbing Zhang, Ming‐Hsien Lee

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A 3 BBi(P 2 O 7 ) 2 (A = Rb, Cs; B = Pb, Ba): Isovalent Cation Substitution to Sustain Large Second-Harmonic Generation ResponsesOriginalBorates: A Rich Source for Optical Materials1089ACs 5 Bi 4 (PO 4 ) 2 (P 2 O 7 ) 3 (A = K, Rb and Cs) with two kinds of isolated P–O groups designed by dimensional reduction theory6Ba 4 Ca(B 2 O 5 ) 2 F 2 : π-conjugation of B 2 O 5 in the planar pentagonal layer achieving large second harmonic generation of pyro -borate34RbMo 2 P 3 O 14 with large birefringence mainly induced by highly distorted [MoO 6 ] in uncommon [Mo 2 P 3 O 14 ] ∞ layers9Synthesis, characterization and theoretical investigation of a new chalcohalide, Ba 4 GaS 4 F 311To improve the key properties of nonlinear optical crystals assembled with tetrahedral functional building units46Ultraviolet nonlinear optical crystals A 3 SrBi(P 2 O 7 ) 2 (A = K, Rb) with large second harmonic generation responses15Ba3Sb2(PO4)4 and Cd3Sb2(PO4)4(H2O)2: Two New Antimonous Phosphates with Distinct [Sb(PO4)2] Structure Types and Enhanced Birefringence37Different mechanism of stereochemical activity and birefringence in post-transition metal halides: A first-principles investigation1UV Solar‐Blind‐Region Phase‐Matchable Optical Nonlinearity and Anisotropy in a π‐Conjugated Cation‐Containing Phosphate196UV Solar‐Blind‐Region Phase‐Matchable Optical Nonlinearity and Anisotropy in a π‐Conjugated Cation‐Containing Phosphate28X-Ray Diffraction and Infrared Spectroscopy Data Review Analyses of the Calcium Phosphates16Hydrogen‐Bond‐Driven Synergistically Enhanced Hyperpolarizability: Chiral Coordination Polymers with Nonpolar Structures Exhibiting Unusually Strong Second‐Harmonic Generation87Hydrogen‐Bond‐Driven Synergistically Enhanced Hyperpolarizability: Chiral Coordination Polymers with Nonpolar Structures Exhibiting Unusually Strong Second‐Harmonic Generation19Sr2Pb(BeB5O10)(BO3): An Excellent Ultraviolet Nonlinear-Optical Beryllium Borate by the Pb-Modified Construction of a Conjugated System and Lone-Pair Effect14Tetrafluoroborate-Monofluorophosphate (NH4)3[PO3F][BF4]: First Member of Oxyfluoride with B–F and P–F Bonds16Tin(II)-Induced Large Birefringence Enhancement in Metal Phosphates22AAl3P6O20 (A = Rb, Cs): Two deep-ultraviolet transparent nonlinear optical materials designed by aliovalent substitution11Band gap modulation and nonlinear optical properties of quaternary tellurates Li 2 GeTeO 613K 2 S 4 O 6 : improving birefringence and nonlinear optical properties with the [O 3 S–S–S–SO 3 ] 2− group5Li 6.58 Na 7.43 Sr 4 (B 9 O 18 )(B 12 O 24 )Cl: unprecedented combination of the largest two highly polymerized isolated B–O clusters with novel isolated B 9 O 18 FBB18Sn 9O 4Br 9X (X = Cl, Br): Two New Sn(II) Oxyhalides Exhibiting Large Birefringence Derived from Highly Distortive Polyhedra of Lone Pair Cations0Variable dimensionality of the anion framework in four new borophosphates and fluoroborophosphates with short cutoff edges13Finding the First Squarates Nonlinear Optical Crystal NaHC4O4·H2O with Strong Second Harmonic Generation and Giant Birefringence56One-Side Capping in Two-Dimensional WO 3 -Type Materials Leading to Strong Second-Harmonic Response29Lone Pair-Driven Enhancement of Birefringence in Polar Alkali Metal Antimony Phosphates46Two Metal Phosphate Nonlinear Optical Materials Simultaneously Exhibiting Ultraviolet Transparence and a Large Birefringence50[C(NH2)3]2Zn(CO3)2: A Guanidinium-Templated Ultraviolet Nonlinear Optical Material20Difluoro(oxalato)borates as Short-Wavelength Optical Crystals with Bifunctional [BF 2 C 2 O 4 ] Units38From Phosphate Fluoride to Fluorophosphate: Design of Novel Ultraviolet/Deep-Ultraviolet Nonlinear Optical Materials for BePO3F with Optical Property Enhancement34NaB3O4F(OH): A Hydroxyfluorooxoborate with One-Dimensional Chain Featuring Large Birefringence and Short Ultraviolet Cutoff Edge5NaK5Zn2(B5O10)2 and β-K3ZnB5O10: Two Zincoborates with Deep-UV Cutoff Edge9Cs2B4O5(OH)4: A new hydrated borate with a short UV cutoff edge2Rb 2 CdSi 4 S 10 : novel [Si 4 S 10 ] T2-supertetrahedra-contained infrared nonlinear optical material with large band gap79LiNaB6O9F2: A Promising UV NLO Crystal Having Fluorine‐Directed Optimal Performances and Double Interpenetrating 3[B6O9F2]∞ Networks33A new infrared nonlinear optical material BaZnGeS 4 with a wide band gap and large nonlinear optical response34KRb 2 (NO 3 ) 2 Cl: a new birefringent crystal exhibiting a perovskite-related framework and a short cutoff edge6MB 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 edge2Modulating optical performance by phase transition in a nonlinear optical material β-Li 2 RbBi(PO 4 ) 28Recent progress on sulfide infrared nonlinear optical materials with large SHG response and wide band gap26Searching for silicate nonlinear optical materials by combining calculation and experiment17Single crystal growth and phase transition mechanism of KCsMoP 2 O 9 with efficient second harmonic generation via the emerging additional periodic phase technology4Structure and optical property evolution in PbM(PO 4 )X (M = Zn, Sn; X = halogen): SHG effect and birefringence21Synthesis and characterization of Cs 2 Zn 4 V 4 O 15 —a new vanadate in the Cs–Zn–V–O quaternary system5Synthesis, structure and characterization of Cd 2 TeO 3 Cl 2 with unprecedented [Cd 2 O 6 Cl 4 ] octahedral dimers5A Rare‐Earth Selenite with Unexpectedly Well‐Balanced Ultraviolet Nonlinear Optical Functionality, Sc(HSeO 3 ) 331Controlling 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 response7Li3B8O13X (X = Cl and Br): Two New Noncentrosymmetric Crystals with Large Birefringence Induced by BO3 Units18Sn9O4Br9X (X = Cl, Br): Two new Sn(II) oxyhalides exhibiting large birefringence derived from highly distortive polyhedra of lone pair cations9Four New Sb‐based Orthophosphates: Cation Regulation to Investigate Diversified Structural Architecture1Stereochemically Active Tin(II)‐Induced Enhancement of Birefringence in SnIISnIV(PO4)2 and SrSn(PO4)PO2(OH)23Phosphates with Two Types of Isolated P–O Groups: Noncentrosymmetric Na 6 Sr 2 Bi 3 (PO 4 )(P 2 O 7 ) 4 and Centrosymmetric Cs 2 CaBi 2 (PO 4 ) 2 (P 2 O 7 )5Na2Mg2P2O7F2: A new diphosphate of the cuspidine family without disorder designed by targeted structural modulation1Improved Birefringence Activated by Tetrahedra Decorated with a Single Linear Unit38Improved Birefringence Activated by Tetrahedra Decorated with a Single Linear Unit1Halide-Induced Band Gap Enhancement from Ba2SnSe4 to KBa2SnSe4Cl2Zn 2 HgP 2 S 8 : A Wide Bandgap Hg‐Based Infrared Nonlinear Optical Material with Large Second‐Harmonic Generation Response75Quadruple‐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 Birefringence2A survey of stereoactive oxysalts for linear and nonlinear optical applications40Deep-ultraviolet (DUV) nonlinear optical (NLO) crystals: An application in photonic technologies29Rare-Earth Scandium Borate Fluoride with a Deep-Ultraviolet Cutoff Edge12Double alkaline earth metals sulfide SrMgGeS4 with high laser-induced damage threshold and strong second-harmonic generation29Stereochemically Active Lone-Pair Containing Metal Substitution in Polar Axis toward a Giant Phase-Matchable Optical Nonlinear Silicate Crystal Li 3 (OH)PbSiO 463Hydroxyl-Driven Enhanced Birefringence in Borophosphates3Two noncentrosymmetric alkali metal phosphates MZnPO4 (M = Rb, Cs) with honeycomb-like structures8Achieving strong second harmonic generation effects induced via dimensional increase of PbX 6 octahedra and halogen substitutes in (C 10 H 11 N 3 )PbX 4 (X = Cl or Br)26Hydrogen bonding bolstered head-to-tail ligation of functional chromophores in a 0D SbF 3 ·glycine adduct for a short-wave ultraviolet nonlinear optical material32Large optical anisotropy in noncentrosymmetric phosphate with pseudo 2D intercalated layer16Design of Deep-Ultraviolet Zero-Order Waveplate Materials by Rational Assembly of [AlO2F4] and [SO4] Groups9Exceptional Optical Anisotropy Enhancement Achieved Through Dual‐Ions Cosubstitution Strategy in Novel Hybrid Bismuth Halides23From ZnF2 to ZnF2(H2O)4: Partial Substitution Achieves Structural Transformation and Nonlinear Optical Activity while Keeping Short Ultraviolet Cutoff Edge19Unearthing Superior Inorganic UV Second‐Order Nonlinear Optical Materials: A Mineral‐Inspired Method Integrating First‐Principles High‐Throughput Screening and Crystal Engineering124Unearthing Superior Inorganic UV Second‐Order Nonlinear Optical Materials: A Mineral‐Inspired Method Integrating First‐Principles High‐Throughput Screening and Crystal Engineering4Design of deep-ultraviolet zero-order waveplate materials using LiB3O5 as the template8Li2B5O8Cl: A New Borate Chloride with Interpenetrating 3D B–O Frameworks Enriching Structural Chemistry of Borate0The electronic structures and optical properties induced by spin-orbit-coupling in LiPbPO4 compound6Effect of synthesis conditions on the thermoluminescence of Li9Mg3[PO4]4F3 fluorophosphate6Enhanced 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 Construction116[C(NH2)3]10(MoO3)10(PO4)2(HPO4)2·5H2O: Synergy effect of multiple functional units results in significant birefringence10Bi(SO4)F·H2O and Bi(SO4)(NO3)·3H2O: Chemical Substitution-Induced Birefringence Enhancement in Bismuth Sulfates6The Directional Design of the Quasi‐Phase‐Matching Short‐Wave Ultraviolet Nonlinear Optical Crystal25Activating Lattice Oxygen Oxidation Mechanism in Asymmetric [IrO6] Octahedra of Ir‐Based Oxides Toward Superior Acidic Electrochemical Water Oxidation14Na(C2H10N2)2[Zn3(PO4)2(H0.5PO4)]2: A Short-Wave Ultraviolet Open-Framework Zincophosphate Exhibiting Substantial Optical Dispersion Ability4Structure and optical properties of alkali rare-earth double phosphates of M3RE(PO4)2 (M = K, Rb; RE = Y, La, and Lu)4Spectroscopic studies and Non-Linear optical response through C/N replacement and modulation of electron Donor/Acceptor Units on naphthyridine derivatives24Deep 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 response41D Bi ribbon/[PO 4 ] synergy-driven bismuth phosphates for ultraviolet nonlinear optical crystals with large SHG and birefringence0BaAlPO 4 F 2 : structure and properties of the first barium fluoroaluminophosphate with the mixed anion group [Al 2 PO 8 F 5 ]1M 2 Al 2 Ti(PO 4 ) 4 (M = Rb, Cs): synthesis and optical property investigation of two titanium phosphates with a dissimilar structural configuration2Multi-site occupied Cs2Ba3(P2O7)2:Eu2+ phosphor with blue-green dual emission for full-spectrum lighting2Tuning the Anionic Configuration in ASc2(P2O7)2 (A = Ba, Pb) through A-Site Cationic Coordination Engineering0KF·[SO 2 (NH 2 ) 2 ]: the First Deep‐Ultraviolet Transparent Sulfonamide Fluoride Nonlinear Optical Crystal with Novel Cairo Pentagonal Structure13KF·[SO 2 (NH 2 ) 2 ]: the First Deep‐Ultraviolet Transparent Sulfonamide Fluoride Nonlinear Optical Crystal with Novel Cairo Pentagonal Structure5Growth, structure and optical properties of PbBi3PO8 crystals0The different response in band structures and optical properties induced by spin-orbit coupling in Ba3X2(PO4)4 (X = Sb and Bi): A first-principles investigation0[Al(H 2 O) 6 ](NO 3 )Cl 2 : achieving parallel arrangement of functional units and birefringence enhancement through free halogen-mediated structural regulation0Polyhedral replacement-guided design of Ce3MnGaSe7 featuring strong second-harmonic genera-tion and high laser-induced damage threshold0Enhanced tripling-performance in [C(NH2)3]4P2O7·H2O as UV nonlinear optical material due to π-conjugated cation and hydrogen bonding intervention1The Power of Pnictogen Bond: As─As Linkages Drive Wide Bandgap, Strong NLO Response and Large Birefringence in SrGa 3 Si 4 As 115The Power of Pnictogen Bond: As─As Linkages Drive Wide Bandgap, Strong NLO Response and Large Birefringence in SrGa 3 Si 4 As 110Exceptional Solar‐Blind Birefringence Engineered by Complementary Hydrogen‐Bond Ordering of π‐Conjugated Units0Three Rare‐Earth Metal Borates Synthesized via a Cation Substitution Strategy as Potential Zero‐Order Waveplate Materials0

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