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RESEARCH PAPER · Chemistry of Materials · 2020

Partial Isovalent Anion Substitution to Access Remarkable Second-Harmonic Generation Response: A Generic and Effective Strategy for Design of Infrared Nonlinear Optical Materials

Mao‐Yin Ran, Zuju Ma, Hong Chen, Bingxuan Li, Xintao Wu, Hua Lin, Qi‐Long Zhu

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Partial Isovalent Anion Substitution to Access Remarkable Second-Harmonic Generation Response: A Generic and Effective Strategy for Design of Infrared Nonlinear Optical MaterialsOriginalA new type of novel salt-inclusion chalcogenide with ultralow thermal conductivity14New quaternary chalcogenide Ba 4 HgAs 2 S 10 originating from the combination of linear [HgS 2 ] 2− and tetrahedral [AsS 4 ] 3− modules8Inherent laws between tetrahedral arrangement pattern and optical performance in tetrahedron-based mid-infrared nonlinear optical materials130Salt-Inclusion Chalcogenide [Ba4Cl2][ZnGa4S10]: Rational Design of an IR Nonlinear Optical Material with Superior Comprehensive Performance Derived from AgGaS2134Pb 18 O 8 Cl 15 I 5 : A Polar Lead Mixed Oxyhalide with Unprecedented Architecture and Excellent Infrared Nonlinear Optical Properties165Pb18O8Cl15I5: A Polar Lead Mixed Oxyhalide with Unprecedented Architecture and Excellent Infrared Nonlinear Optical Properties29Recent Advances in Oxide‐based Nonlinear Optical Materials with Wide Infrared Transparency Beyond 6 μm38Two Mixed-Anion Units of [GeOSe3] and [GeO3S] Originating from Partial Isovalent Anion Substitution and Inducing Moderate Second Harmonic Generation Response and Large Birefringence55Sr6(Li2Cd)A4S16 (A = Ge, Sn): How to Go beyond the Band Gap Limitation via Site-Specific Modification40Ultralow thermal conductivity in the quaternary semiconducting chalcogenide Cs 4 [Ho 26 Cd 7 Se 48 ] with an unprecedented closed cavity architecture7From AgGaS 2 to AgHgPS 4 : vacancy defects and highly distorted HgS 4 tetrahedra double-induced remarkable second-harmonic generation response67Chiral Template‐Driven Macroscopic Chirality Control: Structure‐Second‐Harmonic Generation Properties Relationship24Hydrogen-Bond-Assisted Alignment of [MCu(SeO 3 ) 4 Cl(H 2 O)] 4– (M = Fe, Ga) Anionic Layers to Form Two Polar Oxychlorides: Pb 2 MCu(SeO 3 ) 4 Cl(H 2 O)10A 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 tensors31M 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 anions70Recent progress in oxychalcogenides as IR nonlinear optical materials79Zn(NH 3 )CO 3 : a “three-in-one” UV nonlinear optical crystal built by a polar molecule bonding strategy18Structural Modulation from Cu 3 PS 4 to Cu 5 Zn 0.5 P 2 S 8 : Single-Site Aliovalent-Substitution-Driven Second-Harmonic-Generation Enhancement28AXHg3P2S8 (A = Rb, Cs; X = Cl, Br): New Excellent Infrared Nonlinear Optical Materials with Mixed‐Anion Chalcohalide Groups of Trigonal Planar [HgS2X]3− and Tetrahedral [HgS3X]5−58Centrosymmetric or Noncentrosymmetric? Transition Metals Talking in K 2 TGe 3 S 8 (T = Co, Fe)25Transition-metal-based chalcogenides: A rich source of infrared nonlinear optical materials184La 3 Ga 3 Ge 2 S 3 O 10 : An Ultraviolet Nonlinear Optical Oxysulfide Designed by Anion‐Directed Band Gap Engineering63La3Ga3Ge2S3O10: An Ultraviolet Nonlinear Optical Oxysulfide Designed by Anion‐Directed Band Gap Engineering18A Potassium Tungsten Oxyfluoride with Strong Second-Harmonic Generation Response Derived from Anion-Ordered Functional Motif18Highly polarized [GeOTe 3 ] motif-driven structural order promotion and an enhanced second harmonic generation response in the new nonlinear optical oxytelluride Ba 3 Ge 2 O 4 Te 334Complex coordinated functional groups: A great genes for nonlinear optical materials64Structural modification from centrosymmetric Rb 4 Hg 2 Ge 2 S 8 to noncentrosymmetric (Na 3 Rb)Hg 2 Ge 2 S 8 : mixed alkali metals strategy for infrared nonlinear optical material design28Phase Matchability Transformation in the Infrared Nonlinear Optical Materials with Diamond‐Like Frameworks63Bridging oxygen atoms in trigonal prism units driven strong second-harmonic-generation efficiency in Sr 3 Ge 2 O 4 Te 318From oxides to oxysulfides: the mixed-anion GeS 3 O unit induces huge improvement in the nonlinear optical effect and optical anisotropy for potential nonlinear optical materials19Interesting dimensional transition through changing cations as the trigger in multinary thioarsenates displaying variable photocurrent response and optical anisotropy22KNa 0.78 Eu 0.27 In 3.80 B 12 S 12 : a novel hexanary thioborate featuring a B 12 S 12 cluster and diverse InS x ( x = 4, 5, 6) units9Phase 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 of a promising oxychalcogenide infrared nonlinear optical crystal60Rational design via dual-site aliovalent substitution leads to an outstanding IR nonlinear optical material with well-balanced comprehensive properties68Quaternary 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 Substitution22Pb 4 SeBr 6 : A Congruently Melting Mid‐Infrared Nonlinear Optical Material with Excellent Comprehensive Performance39Sr3[SnOSe3][CO3]: A Heteroanionic Nonlinear Optical Material Containing Planar π‐conjugated [CO3] and Heteroleptic [SnOSe3] Anionic Groups78Sr3[SnOSe3][CO3]: A Heteroanionic Nonlinear Optical Material Containing Planar π‐conjugated [CO3] and Heteroleptic [SnOSe3] Anionic Groups7Nonlinear 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)97Heteroanionic Melilite Oxysulfide: A Promising Infrared Nonlinear Optical Candidate with a Strong Second-Harmonic Generation Response, Sufficient Birefringence, and Wide Bandgap65First Investigation of Nonlinear Optical Oxychalcogenide with Three‐Dimensional Anionic Framework and Special Windmill‐Like Functional Motifs †28A comprehensive review on metal chalcogenides with three-dimensional frameworks for infrared nonlinear optical applications114Synthesis, characterization and theoretical calculations of four chiral schiff base materials for second harmonic generation applications7Recent developments on Bi-based oxychalcogenide materials with thermoelectric and optoelectronic applications: an overview33Oxychalcogenides as Promising Ultraviolet Nonlinear Optical Candidates: Experimental and Theoretical Studies of AEGeOS2(AE = Sr and Ba)24Simple yet extraordinary: Super-polyhedra-built 3D chalcogenide framework of Cs5Ga9S16 with excellent infrared nonlinear optical performance29Characterizations and Nonlinear-Optical Properties of Pentanary Transition-Metal Oxysulfide Sr2CoGe2OS626The Antiperovskite‐Type Oxychalcogenides Ae3Q[GeOQ3] (Ae = Ba, Sr; Q = S, Se) with Large Second Harmonic Generation Responses and Wide Band Gaps68Ba5Ga2SiO4S6: a Phase-Matching Nonlinear Optical Oxychalcogenide Design via Structural Regulation Originated from Heteroanion Introduction25Enhanced Second-Harmonic Generation of van der Waals CuInP 2 S 6 via Pressure-Regulated Cationic Displacement61Oxychalcogenides: A Promising Class of Materials for Nonlinear Optical Crystals with Mixed‐Anion Groups35A 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 materials22Anisotropic structure building unit involving diverse chemical bonds: a new opportunity for high-performance second-order NLO materials181Heteroanion-introduction-driven birefringence enhancement in oxychalcogenide Ba 3 M II Ge 3 O 2 S 8 (M II = Mn, Cd)19Melilite oxychalcogenide Sr 2 FeGe 2 OS 6 : a phase-matching IR nonlinear optical material realized by isomorphous substitution30Synthesis, structure and characterization of Cd 2 TeO 3 Cl 2 with unprecedented [Cd 2 O 6 Cl 4 ] octahedral dimers5Fluorooxoborates: 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 optimization133Rational Design of a Rare‐Earth Oxychalcogenide Nd3[Ga3O3S3][Ge2O7] with Superior Infrared Nonlinear Optical Performance64Sr6Ge3OSe11: A Rationally Designed Noncentrosymmetric Oxyselenide with Polar [GeOSe3] Building Blocks16Comprehensive review on multiple mixed-anion ligands, physicochemical performances and application prospects in metal oxysulfides32Host–Guest Symmetry Matching in Two Crystalline Magnesium Sulfate Oxalates Obtained Via a Solvent-Free Route8Recent progress of newly developed functional building units and corresponding nonlinear optical materials14Recent advances in IR nonlinear optical chalcogenides with well-balanced comprehensive performance56Halide-Induced Band Gap Enhancement from Ba2SnSe4 to KBa2SnSe4Cl2A survey of stereoactive oxysalts for linear and nonlinear optical applications40Two Noncentrosymmetric Bismuth Phosphates: Rational Design Synthesis and Optical Properties4LiGa(IO3)4: An Excellent NLO Material with Unprecedented 2D [Ga(IO3)4]∞− Layer Synthesized by Aliovalent Substitution20Mixed Anionic Tetrahedra Guided Design of New Infrared Nonlinear Optical Material Cs 3 Ga 8 S 13 Cl with High Laser‐Induced Damage Threshold26Double 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 Application49Chiral and Polar Duality Design of Heteroanionic Compounds: Sr18Ge9O5S31 Based on [Sr3OGeS3]2+ and [Sr3SGeS3]2+ Groups20Regulating the key performance parameters for Hg-based IR NLO chalcogenides via bandgap engineering strategy26Ga-based IR nonlinear optical materials: Synthesis, structures, and properties65A UV non-hydrogen pure selenite nonlinear optical material for achieving balanced properties through framework-optimized structural transformation41Cation and anion co-partial substitution induced centrosymmetric to noncentrosymmetric structural transformation to construct nonlinear-optical rare-earth oxythiogermanates13Partial 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 oxychalcogenide Eu 2 ZnGe 2 OS 6 : a phase-matching infrared nonlinear optical material with [GeOS 3 ] units7Rare-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 transformation23Polysulfide Anions [S x ] 2− ( x = 2, 3, 4, 5): Promising Functional Building Units for Infrared Nonlinear Optical Materials22Ba10In2Mn11Si3O12S18: First Hexanary Oxychalcogenide Containing an Infrequent Three-Dimensional Noncentrosysmmetric Framework8The first Hg-based oxychalcogenide Sr2HgGe2OS6: Achieving balanced IR nonlinear optical properties through synergistic cation and anion substitution28Synthesis and Properties of La14TME6CuS24O4, Exhibiting Multivalent Spin Chains (TME = Cr, Fe)1Sr2HgGe2OS6: A Hg-Based Oxychalcogenide Infrared Nonlinear Optical Material Exhibiting Favorable Balance between a Large Band Gap and Strong Second Harmonic Generation Response10Recent advances and future perspectives on rare-earth-based nonlinear optical materials with π-conjugated [XO3] (X = B, C, N) units66Ae3[TO3][SnOQ3] (Ae = Sr, Ba; T = Si, Ge; Q = S, Se) and Ba3[CO3][MQ4] (M = Ge, Sn; Q = S, Se): Design and Syntheses of a Series of Heteroanionic Antiperovskite-Type Oxychalcogenides29Realizing Excellent Infrared Nonlinear Optical Performance in Eu-Based Chalcogenides via Rational Cross Substitution Strategy26Balanced IR Nonlinear Optical Performance Achieved by Cation–Anion Module Cosubstitution in V-Based Salt-Inclusion Oxychalcogenides22La 3 (Ga 3 S 3 O 3 )(Si 2 O 7 ): An Oxychalcogenide Demonstrating Ultrawide Optical Bandgap and Favorable Birefringence Propelled by Divergent Anionic Groups6Emergent Mid‐Infrared Nonlinear Optical Candidates With Targeted Balance Performances17Phase transition engineering to break the symmetry of diamond-like chalcogenide for second-order nonlinear optics2Hetero‐Anionic Oxychalcogenides with Structures and Properties Tuned by the O:S Ratio14Strong Second‐Harmonic Generation Responses in Salt‐Inclusion Oxychalcogenides Enabled by the Highly Distorted Polyhedra with Mixed‐Anions4Oxygen‐Substitution Induced High‐Performance Nonlinear Optical Properties: Witnessed by the First Quaternary Oxythiostannate12Zero-Dimensional Oxyselenide Ba12[(Ga2OSe5)3(Si2O7)]: Enhanced Optical Anisotropy through Heteroanionic Engineering4Unravelling the impact of octahedral distortion and non-covalent interactions on the hyperpolarizabilities of Co(II) and Ni(II) coordination complexes with uridine nucleotide11From Centrosymmetric Ca3Ge2O3S4 to Noncentrosymmetric Ca3Ge2O4Se3: A Nonlinear Optical Ca-Based Oxyselenide5A Series of Pentanary Rare-Earth Oxysulfides Obtained by Heterovalent Cation and Anion Cosubstitution Exhibiting Nonlinear Optical Activity and Ultrawide Band Gaps1Synergistic 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 Crystals0A high-performance IR nonlinear optical material Sr 3 MnGe 2 S 8 achieved via partial cation substitution-induced structural transformation2Crystal structures and electronic structures of SrSiSe 3 and BaGeSe 30Achieving phase matching in infrared nonlinear optical crystal Cd3ZnSiS6 via isovalent substitution from Cd4SiS60Circumventing the Eg–SHG trade-off in selenides: Salt-inclusion [X4Br2][MGa4Se10] with concurrent large band gap and strong nonlinear optical response1Heterometallic Ge–O–Sn-Bridged Oxychalcogenides Sr3GeSnO4Q3 (Q = S, Se) with Wide Band Gaps and Moderate Infrared Nonlinear Optical Responses0Investigating Nonlinear Optical and Thermal Properties in Sr2SiSe4 through Noncentrosymmetric Crystal Structure Comparison with Sr2SnSe41

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  4. Salt-Inclusion Chalcogenide [Ba4Cl2][ZnGa4S10]: Rational Design of an IR Nonlinear Optical Material with Superior Comprehensive Performance Derived from AgGaS2

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