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RESEARCH PAPER · Journal of Materials Chemistry C · 2019

Centric-to-acentric structure transformation induced by a stereochemically active lone pair: a new insight for design of IR nonlinear optical materials

Hua Lin, Yanyan Li, Mengyue Li, Zuju Ma, Li‐Ming Wu, Xintao Wu, Qi‐Long Zhu

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Centric-to-acentric structure transformation induced by a stereochemically active lone pair: a new insight for design of IR nonlinear optical materialsOriginalSn 2 Ga 2 S 5 : A Polar Semiconductor with Exceptional Infrared Nonlinear Optical Properties Originating from the Combined Effect of Mixed Asymmetric Building Motifs81Experiment and First-Principles Calculations of A2Mg2TeB2O10 (A = Pb, Ba): Influences of the Cosubstitution on the Structure Transformation and Optical Properties21Hexagonal In2Se3: A Defect Wurtzite-Type Infrared Nonlinear Optical Material with Moderate Birefringence Contributed by Unique InSe5 Unit75Partial Isovalent Anion Substitution to Access Remarkable Second-Harmonic Generation Response: A Generic and Effective Strategy for Design of Infrared Nonlinear Optical Materials114Glassy Flux Protocol to Confine Lead-Free CsSnX3 Nanocrystals into Transparent Solid Medium17“Soft” Alkali Bromide and Iodide Fluxes for Crystal Growth36First non-centrosymmetric antimony chalcogenides containing mixed cations of alkali and alkaline-Earth: Ba14Na4Sb11S31Cl3 featuring unique disorded 43 helical chains of [Sb5S18]21–5Inherent laws between tetrahedral arrangement pattern and optical performance in tetrahedron-based mid-infrared nonlinear optical materials131A modified chalcogenide flux method for confining metal halide nanocrystals into transparent glassy matrix11Ba3[LiSbS2(S2)2Cl2]: The first zero-dimensional (0D) lithium metal thioantimonate featuring molecular anions of [LiSbS2(S2)2Cl2]6–3Ultralow thermal conductivity in the quaternary semiconducting chalcogenide Cs 4 [Ho 26 Cd 7 Se 48 ] with an unprecedented closed cavity architecture7Recent Achievements in Lone-Pair Cation-Based Infrared Second-Order Nonlinear Optical Materials95A 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 tensors31Breaking through the “3.0 eV wall” of energy band gap in mid-infrared nonlinear optical rare earth chalcogenides by charge-transfer engineering145Deep-ultraviolet transparent alkali metal–rare earth metal sulfate NaY(SO 4 ) 2 ·H 2 O as a nonlinear optical crystal: synthesis and characterization28M 2 As 2 Q 5 (M = Ba, Pb; Q = S, Se): a source of infrared nonlinear optical materials with excellent overall performance activated by multiple discrete arsenate anions70Structural diversities in centrosymmetric La 8 S 4 Cl 8 La 12 S 8 Cl 4 [SbS 3 ] 8 and non-centrosymmetric Ln 12 S 8 Cl 8 [SbS 3 ] 4 (Ln = La and Ce): syntheses, crystal and electronic structures, and optical properties10Ternary rare-earth sulfides RE3GaS6 (RE = Ho, Er): Crystal chemistry, second-order nonlinear optical properties and theoretical investigation18Inorganic Chalcogenides: From Zero‐Dimensional Clusters to Three‐Dimensional Frameworks5α-Ca2CdP2 and β-Ca2CdP2: Two Polymorphic Phosphide-Based Infrared Nonlinear Crystals with Distorted NLO-Active Tetrahedral Motifs Realizing Large Second Harmonic Generation Effects and Suitable Band Gaps30Unique Unilateral-Chelated Mode-Induced d–p−π Interaction Enhances Second-Harmonic Generation Response in New Ln3LiMS7 Family41Rb2CuSb7S12: Quaternary Antimony-Rich Semiconductor Featuring a Three-Dimensional Open Framework and Exhibiting an Intriguing Photocurrent Response31Centrosymmetric or Noncentrosymmetric? Transition Metals Talking in K 2 TGe 3 S 8 (T = Co, Fe)25Recent advances in nonlinear optical rare earth structures63Transition-metal-based chalcogenides: A rich source of infrared nonlinear optical materials184CsCu 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 responses17Rational Crystal Structure Design and Nonlinear-Optical Properties of Noncentrosymmetric RbCu2NbS47Interesting dimensional transition through changing cations as the trigger in multinary thioarsenates displaying variable photocurrent response and optical anisotropy22Phase matching achieved by isomorphous substitution in IR nonlinear optical material Ba 2 SnSSi 2 O 7 with an undiscovered [SnO 4 S] functional motif47Rational design via dual-site aliovalent substitution leads to an outstanding IR nonlinear optical material with well-balanced comprehensive properties69Quaternary Noncentrosymmetric Rare-Earth Sulfides Ba4RE2Cd3S10 (RE = Sm, Gd, or Tb): A Joint Experimental and Theoretical Investigation17From 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 Substitution22SrZnSnSe4: A quaternary selenide with large second harmonic generation and birefringence40Ba6(CuxZy)Sn4S16 (Z = Mg, Mn, Zn, Cd, In, Bi, Sn): High Chemical Flexibility Resulting in Good Nonlinear-Optical Properties12CsY(SO4)2·4H2O: A Deep-Ultraviolet Birefringent Crystal Induced by an Edge-Sharing Connection26Nonlinear optical and detonation properties of semiorganic nitrate crystal C6H14N2(NO3)3·H3O8Enhanced Second-Harmonic-Generation Efficiency and Birefringence in Melillite Oxychalcogenides Sr2MGe2OS6 (M = Mn, Zn, and Cd)97A comprehensive review on metal chalcogenides with three-dimensional frameworks for infrared nonlinear optical applications115Simple yet extraordinary: Super-polyhedra-built 3D chalcogenide framework of Cs5Ga9S16 with excellent infrared nonlinear optical performance29Ba5Ga2SiO4S6: a Phase-Matching Nonlinear Optical Oxychalcogenide Design via Structural Regulation Originated from Heteroanion Introduction25Na 2 Ba[Na 2 Sn 2 S 7 ]: Structural Tolerance Factor‐Guided NLO Performance Improvement50Na2Ba[Na2Sn2S7]: Structural Tolerance Factor‐Guided NLO Performance Improvement0A novel bifunctional thioarsenate based on unprecedented molecular [Cd 4 As 8 Se 16 (Se 2 ) 2 ] 8− cluster anions11A unique [Sb 6 O 2 S 13 ] 12− finite chain in oxychalcogenide Ba 6 Sb 6 O 2 S 13 leading to ultra-low thermal conductivity and giant birefringence12An overview of Mg-based IR nonlinear optical materials23Heteroanion-introduction-driven birefringence enhancement in oxychalcogenide Ba 3 M II Ge 3 O 2 S 8 (M II = Mn, Cd)19LaAeAl 3 S 7 (Ae = Ca, Sr): Cairo pentagonal layered thioaluminates achieving a good balance between a strong second harmonic generation response and a wide bandgap23Melilite oxychalcogenide Sr 2 FeGe 2 OS 6 : a phase-matching IR nonlinear optical material realized by isomorphous substitution30Na 6 Sn 3 P 4 S 16 : Sn( ii )-chelated PS 4 groups inspired an ultra-strong SHG response22Stereochemically active lone-pair-driven giant enhancement of birefringence from three-dimensional CsZn 4 Ga 5 Se 12 to two-dimensional CsZnAsSe 319Visualizing 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]2Rational Design of a Rare‐Earth Oxychalcogenide Nd3[Ga3O3S3][Ge2O7] with Superior Infrared Nonlinear Optical Performance64Recent advances in IR nonlinear optical chalcogenides with well-balanced comprehensive performance57Cs4Zn5P6S18I2: the Largest Birefringence in Chalcohalide Achieved by Highly Polarizable Nonlinear Optical Functional Motifs22Protonated 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 Acid9Double alkaline earth metals sulfide SrMgGeS4 with high laser-induced damage threshold and strong second-harmonic generation29Breaking Through the Trade‐Off Between Wide Band Gap and Large SHG Coefficient in Mercury‐Based Chalcogenides for IR Nonlinear Optical Application49Noncentrosymmetric Na6Pb3P4S16 and Centrosymmetric K2MIIP2S6 (MII = Mg and Zn) Displaying Multiple Membered-Ring Configurations and Strong Optical Anisotropy10Regulating the key performance parameters for Hg-based IR NLO chalcogenides via bandgap engineering strategy26Ga-based IR nonlinear optical materials: Synthesis, structures, and properties65Partial substitution with a significant effect: coexistence of a wide band gap and large birefringence in the oxychalcogenide AEGe 2 O 4 Se (AE = Sr and Ba)17Rare-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 transformation23Evaluation and prospect of Mid-Infrared nonlinear optical materials in f0 rare earth (RE = Sc, Y, La) chalcogenides45The first Hg-based oxychalcogenide Sr2HgGe2OS6: Achieving balanced IR nonlinear optical properties through synergistic cation and anion substitution28A Rare Earth Chalcogenide Nonlinear Optical Crystal KLaGeS4: Achieving Good Balance among Band Gap, Second Harmonic Generation Effect, and Birefringence13Recent advances and future perspectives on rare-earth-based nonlinear optical materials with π-conjugated [XO3] (X = B, C, N) units66LiLnGeS 4 (Ln=La−Nd): Designing High Performance Infrared Nonlinear Optical Sulfides through “Band Reformation of AGS”37LiLnGeS 4 (Ln=La−Nd): Designing High Performance Infrared Nonlinear Optical Sulfides through “Band Reformation of AGS”5Chiral Bimetallic Cuprous-Lead Hybrid Iodide Single Crystals toward Occurrence of Second Harmonic Generation3Balanced IR Nonlinear Optical Performance Achieved by Cation–Anion Module Cosubstitution in V-Based Salt-Inclusion Oxychalcogenides22Exploring new horizons in mid-to-far infrared nonlinear optical crystals: the significant potential of trigonal pyramidal [TeS 3 ] 2− functional units18Isovalent cation substitution drives structural transformation and infrared nonlinear optical activity in Eu-based chalcogenides11Stereochemically active lone pair-induced large optical anisotropy in a novel infrared birefringent crystal Ba 2 La 2 Sb 4 S 10 (S 2 )5Structural diversity and photocurrent responses of multi-component chalcogenidometalates8Ionothermal syntheses, structures, and photocurrent responses of two-dimensional layered thiostannates1Non-centrosymmetric Y3FeGaSe7 and Y3Mn0·5SiSe7 with extremely low thermal conductivities2Recent progress in structural design strategies of high-birefringence optical crystals55Synthesis and Crystal Structures of (C4H12N2)[Mn(HSeO3)2Cl2] and [(C4N12N2)2Br]2[Mn(HSeO3)2Br2]—New Representatives of the Modular Family of “Layered Hydroselenites”1Synergistic Enhancement of Band Gap and Optical Anisotropy via Functional-Site Cosubstitution in Antiperovskite-Type Chalcohalides [Ba2K][X][MS4] (M = Ge, Si; X = Cl, Br)2Structure-property relationships in IR nonlinear optical chalcogenides with stereochemically active lone pairs29Metal Chloride‐Iodate Nonlinear Optical Materials via Direct Chlorination of Centrosymmetric Metal Iodate Crystals0Antibonding States Drive Anharmonicity and Low Thermal Conductivity in Edge-Sharing Metal Chalcogenides4van der Waals layered CuInP 2 S 6 as infrared nonlinear optical material1Piperazinium sulfate – selenous acid cocrystal: a new organically templated non-centrosymmetric compound0Coordination chemistry of Sb(III)-based optical crystals: from lone-pair-induced distortion to birefringence and second-harmonic generation0

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  2. Experiment and First-Principles Calculations of A2Mg2TeB2O10 (A = Pb, Ba): Influences of the Cosubstitution on the Structure Transformation and Optical Properties

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  3. Hexagonal In2Se3: A Defect Wurtzite-Type Infrared Nonlinear Optical Material with Moderate Birefringence Contributed by Unique InSe5 Unit

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  8. Inherent laws between tetrahedral arrangement pattern and optical performance in tetrahedron-based mid-infrared nonlinear optical materials

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  9. A modified chalcogenide flux method for confining metal halide nanocrystals into transparent glassy matrix

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  10. Ba3[LiSbS2(S2)2Cl2]: The first zero-dimensional (0D) lithium metal thioantimonate featuring molecular anions of [LiSbS2(S2)2Cl2]6–

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  11. Ultralow thermal conductivity in the quaternary semiconducting chalcogenide Cs 4 [Ho 26 Cd 7 Se 48 ] with an unprecedented closed cavity architecture

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

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  13. A 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 frameworks

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  15. Ba 2 Ge 2 Te 5 : a ternary NLO-active telluride with unusual one-dimensional helical chains and giant second harmonic-generation tensors

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  17. Deep-ultraviolet transparent alkali metal–rare earth metal sulfate NaY(SO 4 ) 2 ·H 2 O as a nonlinear optical crystal: synthesis and characterization

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  18. M 2 As 2 Q 5 (M = Ba, Pb; Q = S, Se): a source of infrared nonlinear optical materials with excellent overall performance activated by multiple discrete arsenate anions

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  19. Structural diversities in centrosymmetric La 8 S 4 Cl 8 La 12 S 8 Cl 4 [SbS 3 ] 8 and non-centrosymmetric Ln 12 S 8 Cl 8 [SbS 3 ] 4 (Ln = La and Ce): syntheses, crystal and electronic structures, and optical properties

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  32. Phase matching achieved by isomorphous substitution in IR nonlinear optical material Ba 2 SnSSi 2 O 7 with an undiscovered [SnO 4 S] functional motif

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  33. Rational design via dual-site aliovalent substitution leads to an outstanding IR nonlinear optical material with well-balanced comprehensive properties

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  34. Quaternary Noncentrosymmetric Rare-Earth Sulfides Ba4RE2Cd3S10 (RE = Sm, Gd, or Tb): A Joint Experimental and Theoretical Investigation

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  35. From 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 Substitution

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  36. SrZnSnSe4: A quaternary selenide with large second harmonic generation and birefringence

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  38. CsY(SO4)2·4H2O: A Deep-Ultraviolet Birefringent Crystal Induced by an Edge-Sharing Connection

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  39. Nonlinear optical and detonation properties of semiorganic nitrate crystal C6H14N2(NO3)3·H3O

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  41. A comprehensive review on metal chalcogenides with three-dimensional frameworks for infrared nonlinear optical applications

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  42. Simple yet extraordinary: Super-polyhedra-built 3D chalcogenide framework of Cs5Ga9S16 with excellent infrared nonlinear optical performance

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  43. Ba5Ga2SiO4S6: a Phase-Matching Nonlinear Optical Oxychalcogenide Design via Structural Regulation Originated from Heteroanion Introduction

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  44. Na 2 Ba[Na 2 Sn 2 S 7 ]: Structural Tolerance Factor‐Guided NLO Performance Improvement

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  45. Na2Ba[Na2Sn2S7]: Structural Tolerance Factor‐Guided NLO Performance Improvement

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  46. A novel bifunctional thioarsenate based on unprecedented molecular [Cd 4 As 8 Se 16 (Se 2 ) 2 ] 8− cluster anions

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  47. A unique [Sb 6 O 2 S 13 ] 12− finite chain in oxychalcogenide Ba 6 Sb 6 O 2 S 13 leading to ultra-low thermal conductivity and giant birefringence

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  48. An overview of Mg-based IR nonlinear optical materials

    Inorganic Chemistry Frontiers · 2023-01-01

    Jiaxiang Zhang, Mao‐Yin Ran, Xin‐Tao Wu, Hua Lin, Qi‐Long Zhu

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  49. Heteroanion-introduction-driven birefringence enhancement in oxychalcogenide Ba 3 M II Ge 3 O 2 S 8 (M II = Mn, Cd)

    Inorganic Chemistry Frontiers · 2023-01-01

    Shenghua Zhou, Mao‐Yin Ran, Wenbo Wei, A-Yang Wang, Xin‐Tao Wu, Hua Lin, Qi‐Long Zhu

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  50. LaAeAl 3 S 7 (Ae = Ca, Sr): Cairo pentagonal layered thioaluminates achieving a good balance between a strong second harmonic generation response and a wide bandgap

    Inorganic Chemistry Frontiers · 2023-01-01

    Jingjing Xu, Kui Wu, Bingbing Zhang, Haohai Yu, Huaijin Zhang

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