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RESEARCH PAPER · Angewandte Chemie International Edition · 2021

Designing A New Infrared Nonlinear Optical Material, β‐BaGa 2 Se 4 Inspired by the Phase Transition of the BaB 2 O 4 (BBO) Crystal

Yu-Jie Zhang, Qiang Bian, Hongping Wu, Hongwei Yu, Zhanggui Hu, Jiyang Wang, Yicheng Wu

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Designing A New Infrared Nonlinear Optical Material, β‐BaGa 2 Se 4 Inspired by the Phase Transition of the BaB 2 O 4 (BBO) CrystalOriginalRational design via dual-site aliovalent substitution leads to an outstanding IR nonlinear optical material with well-balanced comprehensive properties68The exploration of new infrared nonlinear optical crystals based on the polymorphism of BaGa 4 S 731Sr3[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 Groups7NaGa3Se5: An Infrared Nonlinear Optical Material with Balanced Performance Contributed by Complex {[Ga3Se5]−}∞ Anionic Network14The Combination of Structure Prediction and Experiment for the Exploration of Alkali‐Earth Metal‐Contained Chalcopyrite‐Like IR Nonlinear Optical Material104SrZnGeS 4 : A Dual‐Waveband Nonlinear Optical Material with a Transparency Spanning UV/Vis and Far‐IR Spectral Regions88SrZnGeS4: A Dual‐Waveband Nonlinear Optical Material with a Transparency Spanning UV/Vis and Far‐IR Spectral Regions12Ag4SnGe2S7: A Noncentrosymmetric Chalcogenide in I4–II–IV2–VI7 System with Non-Diamond-Like Structure Featuring 1D ∞[SnGe2S8]6– Infinite Chain2AIB3IIC3IIIQ8VI: A New Family for the Design of Infrared Nonlinear Optical Materials by Coupling Octahedra and Tetrahedra Units152AeMg6Ga6S16 (Ae = Ca, Sr, Ba): The First Double Alkaline‐Earth Metal Chalcogenides with Excellent Performances29Rb 2 CdSi 4 S 10 : novel [Si 4 S 10 ] T2-supertetrahedra-contained infrared nonlinear optical material with large band gap79The Antiperovskite‐Type Oxychalcogenides Ae3Q[GeOQ3] (Ae = Ba, Sr; Q = S, Se) with Large Second Harmonic Generation Responses and Wide Band Gaps68Oxychalcogenides: A Promising Class of Materials for Nonlinear Optical Crystals with Mixed‐Anion Groups35γ-P 4 S 3 I 2 : a new metal-free infrared second-order nonlinear optical crystal designed by polymorphism strategy17From BPS 4 to AB 3 P 2 S 10 (A = Na, K): cations inducing dimension reduction and bandgap enlargement7Honeycomb layered topology construction for exceptional long-wave infrared nonlinear optical crystals29Rational Design of a Rare‐Earth Oxychalcogenide Nd3[Ga3O3S3][Ge2O7] with Superior Infrared Nonlinear Optical Performance64Optimal Design of Mid-Infrared Nonlinear-Optical Crystals: From SrZnSnSe 4 to SrZnSiSe 422Bending Effect on the Electronic Properties and Nonlinear Optical Responses of Linear Porphyrin Oligomer3Na3SiS3F: A Wide Bandgap Fluorothiosilicate with Unique [SiS3F] Unit and High Laser‐Induced Damage Threshold39HgB2S4: A d10 Metal Thioborate with Giant Birefringence and Wide Band Gap31Three‐in‐One Strategy Constructing the First High‐Performance Nonlinear Optical Sulfide Crystallizing with the P43 Space Group27[Ba4(S2)][ZnGa4S10]: Design of an Unprecedented Infrared Nonlinear Salt‐Inclusion Chalcogenide with Disulfide‐Bonds36Cs4Zn5P6S18I2: the Largest Birefringence in Chalcohalide Achieved by Highly Polarizable Nonlinear Optical Functional Motifs21Giant Mid‐Infrared Second‐Harmonic Generation Response in a Densely‐Stacked Van Der Waals Transition‐Metal Oxychloride39Giant Mid‐Infrared Second‐Harmonic Generation Response in a Densely‐Stacked Van Der Waals Transition‐Metal Oxychloride8LiGa(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 Threshold26A I B 3 II C 2 III Q 6 VI X VII : A Thioborate Halide Family for Developing Wide Bandgap Infrared Nonlinear Materials by Coupling Planar [BS 3 ] and Polycations25Ga-based IR nonlinear optical materials: Synthesis, structures, and properties65Ba 2 GeF 2 Q 3 (Q = S, Se) and Ba 3 GeF 2 Se 4 : new F-based chalcohalides with enhanced birefringence9Effectively designing infrared nonlinear optical materials with magnetism, MMn 6 Ga 6 S 16 (M = Ca, Sr, Ba, and Pb), aided by stable open frameworks13New ultraviolet transparent rare-earth borates with enhanced birefringence induced by cation chemical substitution15Wide band gap selenide infrared nonlinear optical materials A II Mg 6 Ga 6 Se 16 with strong SHG responses and high laser-induced damage thresholds31Molecular Crystals Constructed by Polar Molecular Cages: A Promising System for Exploring High‐performance Infrared Nonlinear Optical Crystals6Molecular Crystals Constructed by Polar Molecular Cages: A Promising System for Exploring High‐performance Infrared Nonlinear Optical Crystals34Cs 3 In(In 4 Se 7 )(P 2 Se 6 ): A Multi‐Chromophore Chalcogenide with Excellent Nonlinear Optical Property Designed by Group Grafting55Cs3In(In4Se7)(P2Se6): A Multi‐Chromophore Chalcogenide with Excellent Nonlinear Optical Property Designed by Group Grafting2LaMg6Ga6S16: a chemical stable divalent lanthanide chalcogenide70Assembly of π‐Conjugated [B 3 O 6 ] Units by Mer‐Isomer [YO 3 F 3 ] Octahedra to Design a UV Nonlinear Optical Material, Cs 2 YB 3 O 6 F 211Assembly of π‐Conjugated [B3O6] Units by Mer‐Isomer [YO3F3] Octahedra to Design a UV Nonlinear Optical Material, Cs2YB3O6F297Zn(C6H4NO2)2·4H2O: A Solar-Blind Birefringent Crystal5A Rare Earth Chalcogenide Nonlinear Optical Crystal KLaGeS4: Achieving Good Balance among Band Gap, Second Harmonic Generation Effect, and Birefringence12Structure‐Prediction‐Oriented Synthesis of Thiophosphates as Promising Infrared Nonlinear Optical Materials24Structure‐Prediction‐Oriented Synthesis of Thiophosphates as Promising Infrared Nonlinear Optical Materials1Unraveling the Deep‐Level Defects Induced Optical Losses in LilnSe2 Crystal toward Enhancement of Mid‐Infrared Laser Radiation13Ba2ScBSi2O9: A Mixed-Coordination Borosilicate with a Low B/Si Ratio Exhibiting Enhanced Second Harmonic Generation Response7LiLnGeS 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”5ACuGa 6 S 10 (A = Rb, Cs): Design and Synthesis of Two New Cavity‐Chalcopyrite Chalcogenides Based on “Iterative Substitution” Strategy4Designing infrared nonlinear optical crystals, Sr 2 MgSn 2 OS 6 and Sr 2 SnGa 2 OS 6 , with hybrid anionic frameworks via a double substitution strategy4NaCaGa 3 S 6 : a mixed alkali metal and alkaline earth metal sulfide with a distinctive [Ga 5 S 10 ] ∞ layered framework0Phase transition engineering to break the symmetry of diamond-like chalcogenide for second-order nonlinear optics2Prismatic crystal field stabilized divalent rare-earth chalcogenide REIIBII6CIII6QVI16 with bifunctionality30磷属红外非线性光学晶体带隙调控的可能策略（特邀）5Pb 4 O 3 I 2 : A Lead Oxyhalide IR Optical Crystal with an Unprecedented 1 ∞ [O 3 Pb 4 ] Chain Featuring a Wide Transmittance Range and Large Birefringence3Synergically Assembling Advantageous Groups toward High‐Performance Infrared Nonlinear Optical Materials A II CdSiSe 4 (A II = Sr, Ba)40Cation Equivalent Multisubstitution Realizing Structure Transformation and Balanced Nonlinear Optical Performance of Quaternary Eu-Based Chalcogenides8KYSiSe 4 : A Rare-Earth Selenide Infrared Nonlinear Optical Crystal with Wide Infrared Transparency and Well-Balanced E g and SHG Response9Diamond-Like HgIn2Q4 (Q = Se, Te) Synthesized by Flux-Assisted Boron-Chalcogen Method Exhibit Noteworthy Nonlinear Optical Properties Contributed by Three Types of Tetrahedral Motifs8SrZnSiS4: Shattering the 4.0 eV Threshold toward Dual-Optimized Bandgap and Second-Harmonic Generation5Alkaline Earth-Based Ternary Chalcogenide Nanocrystals: Cadmium- and Lead-Free Optical Materials5Modulating Nonlinear Optical Performances in α/β-SnGa2GeS6 Polymorphs via Atomic Coordination Engineering1LiPb 3 GeS 4 Cl 3 : Quasi‐T 2 ‐Supertetrahedral 3D Framework Enabling Superior Optical Performance14LiPb 3 GeS 4 Cl 3 : Quasi‐T 2 ‐Supertetrahedral 3D Framework Enabling Superior Optical Performance3Cation regulation achieves symmetry breaking: from centrosymmetric M 2 Cs 2 B 10 O 17 (M = Na, K) to noncentrosymmetric Na 3 CsB 10 O 172[Rb 4 Cl][Cd 11 In 9 Se 26 ]: a salt inclusion chalcogenide with a diamond-like framework for infrared nonlinear optics0Selenium-Based Molecular Cage Crystal β-P 4 Se 3 Br 2 : A Promising Candidate for Infrared Nonlinear Optical Applications1Topology-Guided Discovery of BaIn 2 Si 7 P 12 : A Quaternary Diamond-like Framework Phosphide with Giant Second-Harmonic Generation and High Laser-Induced Damage Threshold22Ba 4 CdGa 2 S 6 F 4 : A Chalcohalide Birefringent Crystal with Large Band Gap Designed by the Cation and Anion Cosubstitution Strategy2Entropy‐Driven Structural Modulation Enables High‐Efficiency Nonlinear Optical Performance in Defective Wurtzite Selenides2Achieving Excellent Nonlinear Optics in α ‑Ba 2 Ge 4 S 10 via Flux‑Induced Symmetry Breaking1Mid‐ to Far‐Infrared Nonlinear Optical Crystals: Design Strategies, Structure–Property Relationships and Engineering Prospects0AVP2S7 (A = K, Rb): Dual-Optimized Infrared Nonlinear Optical Thiophosphates via Heterovalent-Substitution-Driven Symmetry Breaking and Reinforced Interlayer Interactions0

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  2. The exploration of new infrared nonlinear optical crystals based on the polymorphism of BaGa 4 S 7

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  12. Rb 2 CdSi 4 S 10 : novel [Si 4 S 10 ] T2-supertetrahedra-contained infrared nonlinear optical material with large band gap

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  14. Oxychalcogenides: A Promising Class of Materials for Nonlinear Optical Crystals with Mixed‐Anion Groups

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  15. γ-P 4 S 3 I 2 : a new metal-free infrared second-order nonlinear optical crystal designed by polymorphism strategy

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  18. Rational Design of a Rare‐Earth Oxychalcogenide Nd3[Ga3O3S3][Ge2O7] with Superior Infrared Nonlinear Optical Performance

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  49. LiLnGeS 4 (Ln=La−Nd): Designing High Performance Infrared Nonlinear Optical Sulfides through “Band Reformation of AGS”

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  50. LiLnGeS 4 (Ln=La−Nd): Designing High Performance Infrared Nonlinear Optical Sulfides through “Band Reformation of AGS”

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    Qianqian Liu, Xin Liu, Mei-Ze Li, Rui‐Xi Wang, Bingxuan Li, Li‐Ming Wu, Ling Chen

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