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RESEARCH PAPER · Crystal Growth & Design · 2020

Recent Achievements in Lone-Pair Cation-Based Infrared Second-Order Nonlinear Optical Materials

Mei Yan, Huaiguo Xue, Sheng‐Ping Guo

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Recent Achievements in Lone-Pair Cation-Based Infrared Second-Order Nonlinear Optical MaterialsOriginalA 3 Mn 2 Sb 3 S 8 (A = K and Rb): a new type of multifunctional infrared nonlinear optical material based on unique three-dimensional open frameworks53Aliovalent-cation-substitution-induced structure transformation: a new path toward high-performance IR nonlinear optical materials47Ba 2 Ge 2 Te 5 : a ternary NLO-active telluride with unusual one-dimensional helical chains and giant second harmonic-generation tensors31Recent progress in oxychalcogenides as IR nonlinear optical materials79AZn4Ga5Se12 (A = K, Rb, or Cs): Infrared Nonlinear Optical Materials with Simultaneous Large Second Harmonic Generation Responses and High Laser-Induced Damage Thresholds34Transition-metal-based chalcogenides: A rich source of infrared nonlinear optical materials184The Rise of Infrared Nonlinear Optical Pnictides: Advances and Outlooks36CsCu 3 SbS 4 : rational design of a two-dimensional layered material with giant birefringence derived from Cu 3 SbS 442Cs 3 CuAs 4 Q 8 (Q = S, Se): unique two-dimensional layered inorganic thioarsenates with the lowest Cu-to-As ratio and remarkable photocurrent responses17Complex Structural Disorder in a Polar Orthorhombic Perovskite Observed through the Maximum Entropy Method/Rietveld Technique6Sn7Br10S2: The First Ternary Halogen‐Rich Chalcohalide Exhibiting a Chiral Structure and Pronounced Nonlinear Optical Properties24Sn7Br10S2: The First Ternary Halogen‐Rich Chalcohalide Exhibiting a Chiral Structure and Pronounced Nonlinear Optical Properties146A Keggin-type polyoxomolybdate-based crystalline material formed by hydrothermal transformation: photo/electro-catalytic properties and mechanism study21Alkali metal partial substitution-induced improved second-harmonic generation and enhanced laser-induced damage threshold for Ag-based sulfides21Interesting dimensional transition through changing cations as the trigger in multinary thioarsenates displaying variable photocurrent response and optical anisotropy22Pb 3 SBrI 3 : the first Pb-based chalcohalide with multiple halogens features a unique two-dimensional structure composed of diverse Pb-centered polyhedra12Unprecedented mid-infrared nonlinear optical materials achieved by crystal structure engineering, a case study of (KX)P 2 S 6 (X = Sb, Bi, Ba)59Lead Tellurite Crystals BaPbTe2O6 and PbVTeO5F with Large Nonlinear-/Linear-Optical Responses due to Active Lone Pairs and Distorted Octahedra20Quaternary Noncentrosymmetric Rare-Earth Sulfides Ba4RE2Cd3S10 (RE = Sm, Gd, or Tb): A Joint Experimental and Theoretical Investigation17HgTeO2F(OH): A Nonlinear Optical Oxyfluoride Constructed of Active [TeO2F(OH)]2– Pyramids and V-Shaped [HgO2]2– Groups36From Cc to P 6 3 mc : Structural Variation in La 3 S 2 Cl 2 [SbS 3 ] and La 3 OSCl 2 [SbS 3 ] Induced by the Isovalent Anion Substitution22Polar lanthanide copper iodates LnCu(IO3)5 (Ln = La, Ce, Pr, and Nd): Synthesis, crystal structure and characterization6K3ZrF4(SbF4)(SbF5) and K8(ZrF6)(Sb2Zr2F20): Two Zirconium Fluoroantimonites with Low Dimensional Structures and Wide Transparency Range12Cooperative Enhancement of Second Harmonic Generation in an Organic–Inorganic Hybrid Antimony Halide63Ba2MAsQ5 (Q = S and Se) Family of Polar Structures with Large Second Harmonic Generation and Phase Matchability23RbBiP2S6: A Promising IR Nonlinear Optical Material with a Giant Second-Harmonic Generation Response Designed by Aliovalent Substitution80Crystal Growth and Chirality - Technologies and Applications12Improved Polarization in the Sr6Cd2Sb6O7Se10 Oxyselenide through Design of Lateral Sublattices for Efficient Photoelectric Conversion4Improved Polarization in the Sr6Cd2Sb6O7Se10 Oxyselenide through Design of Lateral Sublattices for Efficient Photoelectric Conversion16A comprehensive review on metal chalcogenides with three-dimensional frameworks for infrared nonlinear optical applications115Heteroanionic Control of Exemplary Second-Harmonic Generation and Phase Matchability in 1D LiAsS2–xSex43Crystal Growth of K2HCO3F·H2O with a Very Short Cutoff Edge and Large Birefringence17Pb5(GeO4)(Ge2O7) and Pb3.32Ca1.68(GeO4)(Ge2O7): Two Nonlinear Optical Germanates Induced by Diverse PbOx Polyhedra17PbBi(SeO 3 ) 2 F and Pb 2 Bi(SeO 3 ) 2 Cl 3 : Coexistence of Three Kinds of Stereochemically Active Lone-Pair Cations Exhibiting Excellent Nonlinear Optical Properties57Stereochemically Active Lone Pairs and Nonlinear Optical Properties of Two-Dimensional Multilayered Tin and Germanium Iodide Perovskites116Chalcohalides: A Rising Type of Second‐Order Nonlinear Optical Materials28Organic–Inorganic Hybrid Antimony(III) Halides for Second Harmonic Generation34Syntheses, structures, and characterization of new heteroanionic chalcohalides: Na2Ba17In8Q21F18 (Q = S, Se), KBa2InQ3F2 (Q = S, Se)5Ag-based chalcogenides and derivatives as promising infrared nonlinear optical materials90Recent Advances in Infrared Nonlinear Optical Crystal7A novel bifunctional thioarsenate based on unprecedented molecular [Cd 4 As 8 Se 16 (Se 2 ) 2 ] 8− cluster anions11AIO3·H6TeO6 (A = NH4+, Rb+): Two telluric acid and iodate Co-crystalline compounds with second harmonic generation response4An overview of Mg-based IR nonlinear optical materials23LiVTeO 5 : a mid-infrared nonlinear optical vanadium tellurate crystal exhibiting enhanced second harmonic generation activities and notable birefringence21Recent advances on the synthesis of Sb(III)-based inorganic ultraviolet nonlinear optical materials47Visualizing the alignment of lone pair electrons in La 3 AsS 5 Br 2 and La 5 As 2 S 9 Cl 3 to form an acentric or centrosymmetric structure10Nonlinear Optical Switching Driven by the Lone Pair Electron Effect in a Hybrid Compound: (1S, 4S)‐(+)‐2‐Aza‐5‐oxabicyclo[2.2.1] heptane)2[SbCl5]2C(NH2)3(I3O8)(HI3O8)(H2I2O6)(HIO3)4·3H2O: An Unprecedented Asymmetric Guanidinium Polyiodate with a Strong Second-Harmonic-Generation Response and a Wide Band Gap16SbI3·3S8: A Novel Promising Inorganic Adducts Crystal for Second Harmonic Generation5Fluorooxoborates: A precious treasure of deep-ultraviolet nonlinear optical materials24Recent progress in the design of IR nonlinear optical materials by partial chemical substitution: Structural evolution and performance optimization133A Rare‐Earth Selenite with Unexpectedly Well‐Balanced Ultraviolet Nonlinear Optical Functionality, Sc(HSeO 3 ) 331CsHfF4(IO3): A Hafnium Iodate Exhibiting a Strong Second-Harmonic-Generation Effect and a Wide Band Gap Achieved by Mixed-Ligand Acentric Coordination8[K2PbX][Ga7S12] (X = Cl, Br, I): The First Lead‐Containing Cationic Moieties with Ultrahigh Second‐Harmonic Generation and Band Gaps Exceeding the Criterion of 2.33 eV46Achiral Fluorinated Aromatic Ligands Based Chiral Hybrid Antimony Halides with High‐Efficiency Second‐Harmonic Generation18AgMAsS3 (M = Cd, Hg): Double d10 Cation-Containing Thioarsenites(III) Exhibiting High Photocurrent Response and Moderate Second Harmonic Generation11A two-fold interpenetrated mixed-ligands acentric 3D coordination polymer Zn(OBA)(DIB)·0.5H2O: Topological analysis, fluorescent and second-order NLO properties7Protonated Organic Diamines as Templates for Layered and Microporous Structures: Synthesis, Crystal Chemistry, and Structural Trends among the Compounds Formed in Aqueous Systems Transition Metal Halide or Nitrate–Diamine–Selenious Acid9(C2N2H10)[Co(HPHO3)2Cl2]: the first phosphite analog of layered hydrogen selenites12Ga-based IR nonlinear optical materials: Synthesis, structures, and properties65A defect pyrochlore-like acentric cubic lead titanium-tellurate crystal exhibiting strong second harmonic generation activity and an extended transparent window4Achieving 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)26Pb 6 Ba 3 Si 2 S 8 I 10 : a new thiohalide with a quasi-two-dimensional structure and wide band gap2Rare-earth-based chalcogenides and their derivatives: an encouraging IR nonlinear optical material candidate70RbPbPS 4 : a promising IR nonlinear optical material achieved by lone-pair-cation-substitution-induced structure transformation23Design of Pentanary Mixed-Chalcogenides Ag2In2SiS6–xSex (x = 1, 2) Based on the Bucket Effect: Local Structural Difference and High-Performance Nonlinear-Optical Properties Realized by Partial Congener Substitution5Quantifying Structural Polarization by Continuous Regulation of Lone-Pair Electron Expression in Molecular Crystals52Investigations of structure, thermal stability and optical properties of a new NLO crystal (C3H5N2)+(CF3COO)-0K4Cd3Ge4O13: A Congruent-Melting Germanate Nonlinear Optical Crystal with a Moderate Second-Harmonic Generation Intensity and Broad Transparent Window2The synthesis, structures and characterizations of (C5H12NO)4Cd3Cl10·2H2O and (C5H12NO)2BiCl6·H5O2 crystals0Exploring new horizons in mid-to-far infrared nonlinear optical crystals: the significant potential of trigonal pyramidal [TeS 3 ] 2− functional units18Multifactorial Directed Regulation Of the [Io 3 ] − Units in Praseodymium-Contained Iodates0Structural diversity and photocurrent responses of multi-component chalcogenidometalates8Structural and Spectroscopic Studies of (NH4Cl)[Ni2(H2O)6(Se2O5)Cl2] and (RbBr)[Ni(HSeO3)2(H2SeO3)0.5(H2O)0.5]—New Members of the Transition Metal (Hydro)Selenite-Halide Family0Ionothermal syntheses, structures, and photocurrent responses of two-dimensional layered thiostannates1Rational design of a high-efficiency lead halide organic-inorganic hybrid nonlinear optical switch via molecular engineering5Lone Pair Electron Manipulation: A Promising Avenue for Tuning Properties in Functional Materials3Recent progress in structural design strategies of high-birefringence optical crystals55Exploring Combined Stereochemically Active Lone-Pair and Rattling Effects in Thermoelectrics with Machine Learning Potentials8CsLa(SO 4 ) 2 : A Lanthanum Sulfate Crystal for Nonlinear Optical Applications10Synthesis and Crystal Structures of (C4H12N2)[Mn(HSeO3)2Cl2] and [(C4N12N2)2Br]2[Mn(HSeO3)2Br2]—New Representatives of the Modular Family of “Layered Hydroselenites”1Machine Learning Prediction on Birefringence of Nonlinear Optical Crystals and Polymorphs with Different Birefringence Activities2Multifactorial directed regulation of anionic units in praseodymium-contained iodates1Structure-property relationships in IR nonlinear optical chalcogenides with stereochemically active lone pairs29Maximizing the second-harmonic generation response via coordination-induced localization of nonbonding electrons12Charge-order-induced directional enhancement of non-diagonal second-order nonlinear optical tensor components2Synthesis, crystal chemistry, and semiconducting properties of A 3 B 14 Se 24 (A = Sn/Pb; B = In/Sb/Bi) with step-layered NaCl(111)-type slabs interleaved with NaCl(100)-type ribbons0Helical Mn(II)-based enantiomers based on lactic derivatives with ferroelectric and nonlinear optical properties3Control of Symmetry and Photophysical Properties of Hybrid Antimony Chlorides via Mixed Organic Cations0F−/OH− terminal modification of [B3O6] clusters: Constructing deep-ultraviolet hydroxyfluorooxoborates with tunable optical performance0Antibonding Lone Pairs as Hidden Drivers of Bonding, Dynamics, and Energy Performance0Heterovalent Coexistence‐Driven Symmetry Breaking and Dimensional Evolution: Designing Polar Heart‐Shaped Channels for Exceptional MFIR Nonlinear Optics5Synthesis, Structure, and Thermoelectric Properties of Quaternary Selenides M 2 In 5 Sb 9 Se 23 (M = Sn, Pb) with NaCl-Type Ribbon Motifs0Mixed‐Valence Engineering in Ge 2+ Chalcogenides: Structural Modulation for Balanced Infrared Nonlinear Optics0

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  49. SbI3·3S8: A Novel Promising Inorganic Adducts Crystal for Second Harmonic Generation

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  50. Fluorooxoborates: A precious treasure of deep-ultraviolet nonlinear optical materials

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