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RESEARCH PAPER · Angewandte Chemie International Edition · 2020

Anionic Aliovalent Substitution from Structure Models of ZnS: Novel Defect Diamond‐like Halopnictide Infrared Nonlinear Optical Materials with Wide Band Gaps and Large SHG Effects

Jindong Chen, Chensheng Lin, Dan Zhao, Min Luo, Guang Peng, Bingxuan Li, Shunda Yang, Yingshuang Sun, Ning Ye

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Anionic Aliovalent Substitution from Structure Models of ZnS: Novel Defect Diamond‐like Halopnictide Infrared Nonlinear Optical Materials with Wide Band Gaps and Large SHG EffectsOriginalBreaking through the “3.0 eV wall” of energy band gap in mid-infrared nonlinear optical rare earth chalcogenides by charge-transfer engineering144Halonitrides Zn 2 NX (X=Cl,Br): Novel Mid-Infrared Nonlinear Optical Materials30LiZn(OH)CO3: A Deep‐Ultraviolet Nonlinear Optical Hydroxycarbonate Designed from a Diamond‐like Structure180LiZn(OH)CO3: A Deep‐Ultraviolet Nonlinear Optical Hydroxycarbonate Designed from a Diamond‐like Structure10Mg 2 In 3 Si 2 P 7 : A Quaternary Diamond-like Phosphide Infrared Nonlinear Optical Material Derived from ZnGeP 2130A Congruent‐Melting Mid‐Infrared Nonlinear Optical Vanadate Exhibiting Strong Second‐Harmonic Generation22A Congruent‐Melting Mid‐Infrared Nonlinear Optical Vanadate Exhibiting Strong Second‐Harmonic Generation63Hg 3 P 2 S 8 : A New Promising Infrared Nonlinear Optical Material with a Large Second-Harmonic Generation and a High Laser-Induced Damage Threshold111Giant Second-Harmonic Generation Response and Large Band Gap in the Partially Fluorinated Mid-Infrared Oxide RbTeMo 2 O 8 F149The Rise of Infrared Nonlinear Optical Pnictides: Advances and Outlooks36Designing A New Infrared Nonlinear Optical Material, β‐BaGa 2 Se 4 Inspired by the Phase Transition of the BaB 2 O 4 (BBO) Crystal75Designing A New Infrared Nonlinear Optical Material, β‐BaGa2Se4 Inspired by the Phase Transition of the BaB2O4 (BBO) Crystal13Complex coordinated functional groups: A great genes for nonlinear optical materials64Pnictides: An emerging class of infrared nonlinear optical material candidates47Phase Matchability Transformation in the Infrared Nonlinear Optical Materials with Diamond‐Like Frameworks63Pd and octahedra do not get along: Square planar [PdS4] units in non-centrosymmetric La6PdSi2S1419Phosphogermanate Crystal: A New Ultraviolet–Infrared Nonlinear Optical Crystal with Excellent Optical Performances16Uniform Metal Sulfide@N‐doped Carbon Nanospheres for Sodium Storage: Universal Synthesis Strategy and Superior Performance28Uncovering a Vital Band Gap Mechanism of Pnictides49Non‐Linear Optical Properties of the (RE)3CuGeS7 Family of Compounds16Enhanced Second-Harmonic-Generation Efficiency and Birefringence in Melillite Oxychalcogenides Sr2MGe2OS6 (M = Mn, Zn, and Cd)97The Combination of Structure Prediction and Experiment for the Exploration of Alkali‐Earth Metal‐Contained Chalcopyrite‐Like IR Nonlinear Optical Material104The Kurtz-Perry powder technique revisited: A case study on the importance of reference quality and broadband nonlinear optical measurements using LiInSe232Additive‐Triggered Polar Polymorph Formation: β‐Sc(IO 3 ) 3 , a Promising Next‐Generation Mid‐Infrared Nonlinear Optical Material42Additive‐Triggered Polar Polymorph Formation: β‐Sc(IO3)3, a Promising Next‐Generation Mid‐Infrared Nonlinear Optical Material3The Antiperovskite‐Type Oxychalcogenides Ae3Q[GeOQ3] (Ae = Ba, Sr; Q = S, Se) with Large Second Harmonic Generation Responses and Wide Band Gaps68Honeycomb layered topology construction for exceptional long-wave infrared nonlinear optical crystals29Nitrides: a promising class of nonlinear optical material candidates9Synthesis of chiral high-entropy sulfides for non-linear optical applications13The first polyanion-substitution-driven centrosymmetric-to-noncentrosymmetric structural transformation realizing an excellent nonlinear optical supramolecule [Cd 4 P 2 ][CdBr 4 ]17Polar Phosphorus Chalcogenide Cage Molecules: Enhancement of Nonlinear Optical Properties in Adducts38Polar Phosphorus Chalcogenide Cage Molecules: Enhancement of Nonlinear Optical Properties in Adducts1LnLiSiS4 (Ln = La and Ce): Promising infrared nonlinear optical materials designed by aliovalent substitution from SrCdSiS437Phase Competition and Strong SHG Responses of the Li2MIIMIVSe4 Family: Atom Response Theory Predictions versus Experimental Results24A zinc-conducting chalcogenide electrolyte56Rational Design of a Rare‐Earth Oxychalcogenide Nd3[Ga3O3S3][Ge2O7] with Superior Infrared Nonlinear Optical Performance64Remarkable phase-matchable second-harmonic generation realized by strong polarities of [PbSe3] and [GaSe4] functional motifs in PbGa4Se718Zn 2 HgP 2 S 8 : A Wide Bandgap Hg‐Based Infrared Nonlinear Optical Material with Large Second‐Harmonic Generation Response75BaCu2SiS4: A New Member of the AIIBI2MIVQ4 Chalcogenide Family with a Chiral Crystal Structure6Li, Na, K, Mg, Zn, Al, and Ca Anode Interface Chemistries Developed by Solid‐State Electrolytes115Double alkaline earth metals sulfide SrMgGeS4 with high laser-induced damage threshold and strong second-harmonic generation29Flexible Anionic Groups‐Activated Structure Dissymmetry for Strong Nonlinearity in Ln 2 Ae 3 M IV 3 S 12 Family15Nonlinear Optical Phosphide CuInSi2P4: The Inaugural Member of Diamond-Like Family I–III–IV2–V4 Inspired by ZnGeP216“Three‐in‐One”: A New Hg‐Based Selenide Hg 7 P 2 Se 12 Exhibiting Wide Infrared Transparency Range and Strong Nonlinear Optical Effect80Computer-aided screening of bismuth molybdates nonlinear optical crystals γ -Bi 2 MoO 63Heteroanionic [VO x S 4− x ] groups: tetrahedral units with large birefringence for mid-infrared nonlinear optical crystals9Multi-step cation substitution facilitating the exploration of potential infrared nonlinear optical materials6Halogen-assisted octet binding electrons construction of pnictogens towards wide-bandgap nonlinear optical pnictides17Mixed Anionic M(S/X)6 Polyhedra as Symmetry-Breaking Motifs to Enhance the Infrared Nonlinear Optical Response in Y–M–S–X (M = Ga, Ge; X = Cl, Br)5A Rare Earth Chalcogenide Nonlinear Optical Crystal KLaGeS4: Achieving Good Balance among Band Gap, Second Harmonic Generation Effect, and Birefringence12LiLnGeS 4 (Ln=La−Nd): Designing High Performance Infrared Nonlinear Optical Sulfides through “Band Reformation of AGS”36LiLnGeS 4 (Ln=La−Nd): Designing High Performance Infrared Nonlinear Optical Sulfides through “Band Reformation of AGS”5Achieving strong optical nonlinearity and wide bandgap of pnictides via ionic motif–driven directed assembly of covalent groups39La 3 (Ga 3 S 3 O 3 )(Si 2 O 7 ): An Oxychalcogenide Demonstrating Ultrawide Optical Bandgap and Favorable Birefringence Propelled by Divergent Anionic Groups6Assembly between diverse polycations and diamond-like anionic frameworks in salt-inclusion phosphides enables excellent nonlinear optical properties4Cd5As2Br4: A Ternary Arsenide with Nonlinear Optical Property3Impact of Microstructural Units Configuration and Arrangement on Phase-Matching in Nonlinear Optical KGa5Se8 Crystals9Reinforced Nonlinear Optical Performances Induced by P‐P Homoatomic Bond in Phosphide SrIn 3 Si 4 P 1131Reinforced Nonlinear Optical Performances Induced by P‐P Homoatomic Bond in Phosphide SrIn 3 Si 4 P 116SrZnGeSe 4 : a promising infrared nonlinear optical material with strong second harmonic generation and high laser-induced damage threshold4Vacancy-driven tetrahedral distortion leading to exceptional second harmonic generation3LiPb 3 GeS 4 Cl 3 : Quasi‐T 2 ‐Supertetrahedral 3D Framework Enabling Superior Optical Performance14BaAl2MS6 (M = Si and Ge): the rational construction of diamond-like structures with ultrawide band gap by group-optimization approach6Broadband infrared-transparent crystals enabled by heterologous isomorphic substitution0Harnessing tetrahedral diversity: The path to superior diamond-like IR NLO crystals13Strategic Integration Between Trigonal Architecture Construction and Molecular Polarization Enhancement for Record SHG Effect in Selenates4Design of a High-Performance Infrared Nonlinear Optical Crystal via a Multiple Flexible-Group Synergistic Polarization Strategy10Entropy‐Driven Structural Modulation Enables High‐Efficiency Nonlinear Optical Performance in Defective Wurtzite Selenides2Defect Diamond‐Like d 10 Metal Indium Selenium With Strong Second‐Harmonic Generation and Enhanced Laser‐Induced Damage Threshold2Salt-Inclusion Rare-Earth Chalcogenides: Exploring Infrared Nonlinear Optical Crystals via a Guest-Framework Modulation Strategy0Mid‐ to Far‐Infrared Nonlinear Optical Crystals: Design Strategies, Structure–Property Relationships and Engineering Prospects0First‐Principles Investigation of the Structural, Electronic, Optical, Elastic, and Thermal Properties of Defect Diamond‐Like Hg 3 P 2 S 80CaM 3 Si 4 P 11 (M = Al, Ga): [P 2 ] Motifs‐Modified Quasi‐T 3 Supertetrahedra Drive Superior Infrared Nonlinear Optical Performances1Advances in metal selenite nonlinear optical materials: halogens directed structure modulation and property optimization0Topology‐Preserving Ionic‐Unit Substitution Enables Sphalerite‐Like Phosphides Achieving Superior Infrared Optical Nonlinearity0Variation of Tetrahedrons and Cations Regulates LIDTs in 3D‐DL Structure MIR‐NLO Crystals0Beyond the bandgap bottleneck: structure–property design principles for infrared nonlinear optical phosphides0Homologous lattice coupling drives the formation of tetrahedra-ordered phase exhibiting enhanced optical nonlinearity and band gap0

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  3. LiZn(OH)CO3: A Deep‐Ultraviolet Nonlinear Optical Hydroxycarbonate Designed from a Diamond‐like Structure

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  4. LiZn(OH)CO3: A Deep‐Ultraviolet Nonlinear Optical Hydroxycarbonate Designed from a Diamond‐like Structure

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  5. Mg 2 In 3 Si 2 P 7 : A Quaternary Diamond-like Phosphide Infrared Nonlinear Optical Material Derived from ZnGeP 2

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  9. Giant Second-Harmonic Generation Response and Large Band Gap in the Partially Fluorinated Mid-Infrared Oxide RbTeMo 2 O 8 F

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  15. Phase Matchability Transformation in the Infrared Nonlinear Optical Materials with Diamond‐Like Frameworks

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  16. Pd and octahedra do not get along: Square planar [PdS4] units in non-centrosymmetric La6PdSi2S14

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  17. Phosphogermanate Crystal: A New Ultraviolet–Infrared Nonlinear Optical Crystal with Excellent Optical Performances

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  47. Multi-step cation substitution facilitating the exploration of potential infrared nonlinear optical materials

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  48. Halogen-assisted octet binding electrons construction of pnictogens towards wide-bandgap nonlinear optical pnictides

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  49. Mixed Anionic M(S/X)6 Polyhedra as Symmetry-Breaking Motifs to Enhance the Infrared Nonlinear Optical Response in Y–M–S–X (M = Ga, Ge; X = Cl, Br)

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  50. A Rare Earth Chalcogenide Nonlinear Optical Crystal KLaGeS4: Achieving Good Balance among Band Gap, Second Harmonic Generation Effect, and Birefringence

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