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RESEARCH PAPER · Angewandte Chemie International Edition · 2022

SrZnGeS 4 : A Dual‐Waveband Nonlinear Optical Material with a Transparency Spanning UV/Vis and Far‐IR Spectral Regions

Qianqian Liu, Xin Liu, Li‐Ming Wu, Ling Chen

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SrZnGeS 4 : A Dual‐Waveband Nonlinear Optical Material with a Transparency Spanning UV/Vis and Far‐IR Spectral RegionsOriginalRational design via dual-site aliovalent substitution leads to an outstanding IR nonlinear optical material with well-balanced comprehensive properties69AIB3IIC3IIIQ8VI: A New Family for the Design of Infrared Nonlinear Optical Materials by Coupling Octahedra and Tetrahedra Units152The 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 Groups35Na 2 Ba[Na 2 Sn 2 S 7 ]: Structural Tolerance Factor‐Guided NLO Performance Improvement50Na2Ba[Na2Sn2S7]: Structural Tolerance Factor‐Guided NLO Performance Improvement0A new infrared nonlinear optical material BaZnGeS 4 with a wide band gap and large nonlinear optical response34An overview of Mg-based IR nonlinear optical materials23Anisotropic structure building unit involving diverse chemical bonds: a new opportunity for high-performance second-order NLO materials181Honeycomb layered topology construction for exceptional long-wave infrared nonlinear optical crystals29Revisiting two thiophosphate compounds constituting d 0 transition metal HfP 2 S 6 and d 10 transition metal α-Ag 4 P 2 S 6 as multifunctional materials for combining second harmonic generation response and photocurrent response12The first polyanion-substitution-driven centrosymmetric-to-noncentrosymmetric structural transformation realizing an excellent nonlinear optical supramolecule [Cd 4 P 2 ][CdBr 4 ]17Deep Eutectic Solvents Synthesis of A2Sb(C2O4)Cl3 (A = NH4, K, Rb) with Superior Optical Performance26Unbiased Screening of Novel Infrared Nonlinear Optical Materials with High Thermal Conductivity: Long‐neglected Nitrides and Popular Chalcogenides12Unbiased Screening of Novel Infrared Nonlinear Optical Materials with High Thermal Conductivity: Long‐neglected Nitrides and Popular Chalcogenides48[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 eV46Remarkable phase-matchable second-harmonic generation realized by strong polarities of [PbSe3] and [GaSe4] functional motifs in PbGa4Se718Optimal Design of Mid-Infrared Nonlinear-Optical Crystals: From SrZnSnSe 4 to SrZnSiSe 423Theoretical Prediction‐Assisted Synthesis and Characterization of Infrared Nonlinear Optical Material NaSrBS324Na3SiS3F: A Wide Bandgap Fluorothiosilicate with Unique [SiS3F] Unit and High Laser‐Induced Damage Threshold39Three‐in‐One Strategy Constructing the First High‐Performance Nonlinear Optical Sulfide Crystallizing with the P43 Space Group27Cd2Nb2Te4O15: A Novel Pseudo‐Aurivillius‐Type Tellurite with Unprecedented Nonlinear Optical Properties and Excellent Stability40[Ba4(S2)][ZnGa4S10]: Design of an Unprecedented Infrared Nonlinear Salt‐Inclusion Chalcogenide with Disulfide‐Bonds36Improved Birefringence Activated by Tetrahedra Decorated with a Single Linear Unit38Improved Birefringence Activated by Tetrahedra Decorated with a Single Linear Unit1Halide-Induced Band Gap Enhancement from Ba2SnSe4 to KBa2SnSe4Cl2Zn 2 HgP 2 S 8 : A Wide Bandgap Hg‐Based Infrared Nonlinear Optical Material with Large Second‐Harmonic Generation Response75Three-in-One Tetrahedral Functional Units Constructing Diamondlike Ag2In2SiS3.06Se2.94 with High-Performance Nonlinear-Optical Activity4Mixed Anionic Tetrahedra Guided Design of New Infrared Nonlinear Optical Material Cs 3 Ga 8 S 13 Cl with High Laser‐Induced Damage Threshold26Ca2Ln(BS3)(SiS4) (Ln = La, Ce, and Gd): Mixed Metal Thioborate‐Thiosilicates as Well‐Performed Infrared Nonlinear Optical Materials29A ll HgM IV S 4 (A ll = Sr, Ba, M IV = Si, Ge): A Series of Materials with Large Second Harmonic Generation Response and Wide Band Gaps28Flexible Anionic Groups‐Activated Structure Dissymmetry for Strong Nonlinearity in Ln 2 Ae 3 M IV 3 S 12 Family16Designing Sulfate Crystals with Strong Optical Anisotropy through π‐Conjugated Tailoring51Designing Sulfate Crystals with Strong Optical Anisotropy through π‐Conjugated Tailoring11A 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 Polycations25Ba4Cd2Ge2Te9: A promising infrared functional crystal with large birefringent and photoluminescence properties2Chemical modulation of A I RE III C IV QVI4 family compounds for band gap and optical anisotropy enhancement16Hg 3 AsS 4 X (X = Cl and Br): two Hg-based chalcogenides as long-wave infrared nonlinear optical crystals with superior comprehensive performances33KBa 3 M 2 F 14 Cl (M = Zr, Hf): novel short-wavelength mixed metal halides with the largest second-harmonic generation responses contributed by mixed functional moieties37Multi-step cation substitution facilitating the exploration of potential infrared nonlinear optical materials6Rare-earth-based chalcogenides and their derivatives: an encouraging IR nonlinear optical material candidate70Structural strategy for advancing nonlinear optical effects in 1D-[MX 2 ] ∞ chains: internal distortion and atomic types2Molecular 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 Crystals34Boosted Second Harmonic Generation of a Chiral Hybrid Lead Halide Resonant to Charge Transfer Exciton from Metal Halide Octahedra to Ligand11Boosted Second Harmonic Generation of a Chiral Hybrid Lead Halide Resonant to Charge Transfer Exciton from Metal Halide Octahedra to Ligand48Polysubstitution Induced Centrosymmetric-to-Noncentrosymmetric Structural Transformation and Nonlinear-Optical Behavior: The Case of Na0.45Ag0.55Ga3Se52Mixed 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)5Vacancy‐Induced Extraordinary Second Harmonic Generation Response for Diamond‐Like Cu3PS49Theoretical Prediction of Monolayer BeP 2 O 4 H 4 with Excellent Nonlinear‐Optical Properties in Deep‐Ultraviolet Range6The centrosymmetric to non-centrosymmetric transformation induced by alkaline-earth cations producing infrared nonlinear optical AeMn6Ga6S16 (Ae = Ca, Sr)13LiLnGeS 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”5Computer‐Aided Development of New Nonlinear Optical Materials38Computer‐Aided Development of New Nonlinear Optical Materials14Tin chalcohalide Sn 11 (PS 4 ) 4 I 10 obtained from structural-template-oriented synthesis: exhibiting balanced infrared nonlinear optical performance6Emergent Mid‐Infrared Nonlinear Optical Candidates With Targeted Balance Performances18Rare‐Earth Substitution Induced Symmetry Breaking for The First Sc‐Based Nonlinear Optical Chalcogenide with High‐Performance31A wide band gap selenohalide Cs 9 Si 8 Se 20 Cl with unprecedented [CsSe 7 Cl] mixed anionic units2Ca 2 La(MS 4 )(BS 3 ) (M = Ge/Si and Sn/Si): high-performance infrared nonlinear optical materials designed using an atomic site co-occupancy strategy9Cationic substitution engineering induces a new quaternary chalcogenide in the A–M IIIA –M IVA –Q system for optical crystal applications1Exploring the functional properties of the diamond-like quaternary compound Li 2 ZnGeS 4 for potential energy applications: a theoretical approach2Isovalent cation substitution drives structural transformation and infrared nonlinear optical activity in Eu-based chalcogenides11La 2 ZnGa 2 S 6 O: a melilite-type transition metal oxysulfide achieving a well-balanced nonlinear optical behavior5Partial congener substitution induced wide band gap witnessed in diamond-like chalcogenide ZnHg 2 P 2 S 8 and its second-order nonlinear optical properties3Two-in-one: assembling hybrid supertetrahedra chromophores and achieving high-performance “hexagonal warriors” in nonlinear optical crystals6Discovering Pseudo-Supertetrahedral Functional Units in Salt-Inclusion Nonlinear Optical Material [Ba22(SO4)5][Zn14Ga18S58]14Synergically Assembling Advantageous Groups toward High‐Performance Infrared Nonlinear Optical Materials A II CdSiSe 4 (A II = Sr, Ba)41SrZnGeSe 4 : a promising infrared nonlinear optical material with strong second harmonic generation and high laser-induced damage threshold4Lewis Acidity‐Governed Ion Exchange and Record Birefringence in A′[Ag 3 (PO 3 F) 2 ]11Lewis Acidity‐Governed Ion Exchange and Record Birefringence in A′[Ag 3 (PO 3 F) 2 ]2From Centrosymmetric Eu 2 Ga 2 S 5 to Noncentrosymmetric EuMg 6 Ga 6 S 16 via Introduction of Distorted MgS 6 Octahedron: Featuring Wide Bandgap and Nonlinear Optical Activity3Ba 10 Zn 7 Ga 6 S 26 : Promising Infrared Nonlinear Optical Crystal Exhibiting a High Laser Damage Threshold0SrZnSiS4: Shattering the 4.0 eV Threshold toward Dual-Optimized Bandgap and Second-Harmonic Generation7LiPb 3 GeS 4 Cl 3 : Quasi‐T 2 ‐Supertetrahedral 3D Framework Enabling Superior Optical Performance14KGdSiSe 4 and KGdGeSe 4 : two rare earth-based selenides with wide bandgaps and large nonlinear optical responses0SrMnGeS 4 : A Two-Dimensional Layered Chalcogenide with Magnetic Triangular Lattice0Topology-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 Threshold24From Centrosymmetric Mg 2 GeS 4 to Noncentrosymmetric CdMg 3 Ge 2 S 8 : Cation-Mixing-Driven Symmetry Reduction4Synergistic Distortion Engineering: Activating Nonlinear Optical Response in Quaternary Chalcogenides via Lattice‐Induced [MnS 4 ] Asymmetry2From Coplanarity to Coaxiality: A Linearity-Oriented Design Paradigm for Ultrahigh Ultraviolet Birefringent Inorganic Crystals5Halogen‐Rich Design Strategy: Rational Synthesis of High‐Performance Tetrahedron‐Based Chalcohalides for Advanced Infrared Optical Materials2Gravity‐Field Self‐Regulatory Engineering Enables PbIn 6 Te 10 Nonlinear Optical Crystals Boosting Laser‐Induced Damage Threshold1Mid‐ to Far‐Infrared Nonlinear Optical Crystals: Design Strategies, Structure–Property Relationships and Engineering Prospects0Cation-substitution-driven electronic, nonlinear optical, elastic, and thermal transport properties of layered AeHgGeSe4 (Ae = Ba, Sr): A first-principles study0Cation-Modulated Activation of Linear Units in an Ordered Arrangement Achieves the Largest Optical Anisotropy in Wide-Bandgap Metal Chalcogenides0Mixed‐Valence Engineering in Ge 2+ Chalcogenides: Structural Modulation for Balanced Infrared Nonlinear Optics0[La3Br][GeS4]2: Cationic-Moiety-Guided Strategy Enables Record Birefringence and Broad Optical Window0

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

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  2. AIB3IIC3IIIQ8VI: A New Family for the Design of Infrared Nonlinear Optical Materials by Coupling Octahedra and Tetrahedra Units

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  3. The Antiperovskite‐Type Oxychalcogenides Ae3Q[GeOQ3] (Ae = Ba, Sr; Q = S, Se) with Large Second Harmonic Generation Responses and Wide Band Gaps

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

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

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

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  7. A new infrared nonlinear optical material BaZnGeS 4 with a wide band gap and large nonlinear optical response

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

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  9. Anisotropic structure building unit involving diverse chemical bonds: a new opportunity for high-performance second-order NLO materials

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  10. Honeycomb layered topology construction for exceptional long-wave infrared nonlinear optical crystals

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  11. Revisiting two thiophosphate compounds constituting d 0 transition metal HfP 2 S 6 and d 10 transition metal α-Ag 4 P 2 S 6 as multifunctional materials for combining second harmonic generation response and photocurrent response

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  12. The first polyanion-substitution-driven centrosymmetric-to-noncentrosymmetric structural transformation realizing an excellent nonlinear optical supramolecule [Cd 4 P 2 ][CdBr 4 ]

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  13. Deep Eutectic Solvents Synthesis of A2Sb(C2O4)Cl3 (A = NH4, K, Rb) with Superior Optical Performance

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  14. Unbiased Screening of Novel Infrared Nonlinear Optical Materials with High Thermal Conductivity: Long‐neglected Nitrides and Popular Chalcogenides

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  16. [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 eV

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  17. Remarkable phase-matchable second-harmonic generation realized by strong polarities of [PbSe3] and [GaSe4] functional motifs in PbGa4Se7

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  18. Optimal Design of Mid-Infrared Nonlinear-Optical Crystals: From SrZnSnSe 4 to SrZnSiSe 4

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  19. Theoretical Prediction‐Assisted Synthesis and Characterization of Infrared Nonlinear Optical Material NaSrBS3

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  31. A ll HgM IV S 4 (A ll = Sr, Ba, M IV = Si, Ge): A Series of Materials with Large Second Harmonic Generation Response and Wide Band Gaps

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  32. Flexible Anionic Groups‐Activated Structure Dissymmetry for Strong Nonlinearity in Ln 2 Ae 3 M IV 3 S 12 Family

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  39. KBa 3 M 2 F 14 Cl (M = Zr, Hf): novel short-wavelength mixed metal halides with the largest second-harmonic generation responses contributed by mixed functional moieties

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  41. Rare-earth-based chalcogenides and their derivatives: an encouraging IR nonlinear optical material candidate

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  42. Structural strategy for advancing nonlinear optical effects in 1D-[MX 2 ] ∞ chains: internal distortion and atomic types

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  43. Molecular Crystals Constructed by Polar Molecular Cages: A Promising System for Exploring High‐performance Infrared Nonlinear Optical Crystals

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  44. Molecular Crystals Constructed by Polar Molecular Cages: A Promising System for Exploring High‐performance Infrared Nonlinear Optical Crystals

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  45. Boosted Second Harmonic Generation of a Chiral Hybrid Lead Halide Resonant to Charge Transfer Exciton from Metal Halide Octahedra to Ligand

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  46. Boosted Second Harmonic Generation of a Chiral Hybrid Lead Halide Resonant to Charge Transfer Exciton from Metal Halide Octahedra to Ligand

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  47. Polysubstitution Induced Centrosymmetric-to-Noncentrosymmetric Structural Transformation and Nonlinear-Optical Behavior: The Case of Na0.45Ag0.55Ga3Se5

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  48. 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)

    Chemistry of Materials · 2024-04-01

    Yan Jie Guo, Bin‐Wen Liu, Chao-Hong Xie, Wen‐Fa Chen, Mingxin Li, Xiao‐Ming Jiang, Guo‐Cong Guo

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  49. Vacancy‐Induced Extraordinary Second Harmonic Generation Response for Diamond‐Like Cu3PS4

    Advanced Optical Materials · 2024-04-10

    Weiping Guo, Yudi Fu, Hong‐Hua Cui, Lingyun Li, Yan Yu, Zhong‐Zhen Luo, Zhigang Zou

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  50. Theoretical Prediction of Monolayer BeP 2 O 4 H 4 with Excellent Nonlinear‐Optical Properties in Deep‐Ultraviolet Range

    Small · 2024-06-10

    Xin Liu, Li‐Ming Wu, Lei Kang, Zheshuai Lin, Ling Chen

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