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RESEARCH PAPER · Small · 2023

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

Mao‐Yin Ran, Shenghua Zhou, Wenbo Wei, Bingxuan Li, Xin‐Tao Wu, Hua Lin, Qi‐Long Zhu

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Rational Design of a Rare‐Earth Oxychalcogenide Nd3[Ga3O3S3][Ge2O7] with Superior Infrared Nonlinear Optical PerformanceOriginalA 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 materials22From CdPb 8 (SeO 3 ) 4 Br 10 to Pb 3 (TeO 3 )Br 4 : the first tellurite bromide exhibiting an SHG response and mid-IR transparency21Heteroanion-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 substitution30Stereochemically active lone-pair-driven giant enhancement of birefringence from three-dimensional CsZn 4 Ga 5 Se 12 to two-dimensional CsZnAsSe 319Water‐Assisted Growth of Twisted 3R‐Stacked MoSe 2 Spirals and Its Dramatically Enhanced Second Harmonic Generations12Recent progress of newly developed functional building units and corresponding nonlinear optical materials14AAl(Te 4 O 10 ) (A = Na, Ag) and K 2 Ga 2 (HTe 6 O 16 )(HTeO 3 ): Three Aluminum/Gallium Tellurites with Large Birefringence and Wide Band Gap21Recent advances in IR nonlinear optical chalcogenides with well-balanced comprehensive performance56Cd2Nb2Te4O15: A Novel Pseudo‐Aurivillius‐Type Tellurite with Unprecedented Nonlinear Optical Properties and Excellent Stability40Three-in-One Tetrahedral Functional Units Constructing Diamondlike Ag2In2SiS3.06Se2.94 with High-Performance Nonlinear-Optical Activity4A survey of stereoactive oxysalts for linear and nonlinear optical applications40Four UV Transparent Linear and Nonlinear Optical Materials Explored from Pure Selenite Compounds22Breaking 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+ Groups20Ga-based IR nonlinear optical materials: Synthesis, structures, and properties65“Three‐in‐One”: A New Hg‐Based Selenide Hg 7 P 2 Se 12 Exhibiting Wide Infrared Transparency Range and Strong Nonlinear Optical Effect80A UV non-hydrogen pure selenite nonlinear optical material for achieving balanced properties through framework-optimized structural transformation41Chemical modulation of A I RE III C IV QVI4 family compounds for band gap and optical anisotropy enhancement16Chemical perspectives on heteroanionic compounds: a potential playground for multiferroics7New nonlinear optical oxyfluoride K 2 NbO 2 F 3 with strong pseudo-centrosymmetry, obtained by mild hydrothermal synthesis0Partial 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 transformation23Salt-inclusion sulfides [K 4 Cl][M II 11 In 9 S 26 ] (M II = Zn, Cd) displaying robust nonlinear optical activity4Hg3Se(SeO3)(SO4): A Mixed-Valent Selenium Compound with Mid-Infrared Transmittance Obtained by In Situ Reaction26KREP 2 S 6 (RE = Sm, Gd, Tb, Dy): A Series of Polar Rare-Earth Thiophosphates with High Laser-Induced Damage Thresholds and Moderate Nonlinear-Optical Responses Synergistically Contributed by Isolated P 2 S 6 Units and {[RE 2 S 15 ] 24– } ∞ Layers8Ba10In2Mn11Si3O12S18: First Hexanary Oxychalcogenide Containing an Infrequent Three-Dimensional Noncentrosysmmetric Framework8Reduction of Germanium Oxides–The Mixed-Valence Germanates A2Ge4O7 (A = Na, K)4Hg4(Te2O5)(SO4): A Giant Birefringent Sulfate Crystal Triggered by a Highly Selective Cation153Anhydrous Aluminum Iodate: Strong Second Harmonic Generation Effect Contributed by Unbonded and Antibonding Orbitals3Pentanary Oxythiogermanates Ba3MGe3O2S8 (M = Ca, Zn) Featuring [Ge3O2S8]8– Trimers and {[MGe3O2S8]6–}∞ Chains: Structural Chemistry and Physical Properties4The first Hg-based oxychalcogenide Sr2HgGe2OS6: Achieving balanced IR nonlinear optical properties through synergistic cation and anion substitution28Polymorphism of Niobium Phosphate Bronze Na4Nb8P4O32Deduced by the Packings of Structural Units: A Centrosymmetric Phase7PbBeB2O5: A High-Performance Ultraviolet Nonlinear-Optical Crystal with Functional [BeB2O8]8– Group3Old tree blossoms anew: Research progress on the structures and optical properties of ultraviolet selenites56Ag 2 GeS 3 : A Diamond‐Like Chalcogenide as an IR Nonlinear Optical Material with Outstanding Second‐Harmonic Generation Response28Realizing Excellent Infrared Nonlinear Optical Performance in Eu-Based Chalcogenides via Rational Cross Substitution Strategy26From [Ba3S][GeS4] to [Ba3CO3][MS4] (M = Ge, Sn): Enhancing optical anisotropy in IR birefringent crystals via functional group implantation11Rare-Earth/d10 Dual-Metal Oxychalcogenides as Infrared Nonlinear-Optical Materials10Balanced 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 Performances17Exploring 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 chalcogenides11La 2 ZnGa 2 S 6 O: a melilite-type transition metal oxysulfide achieving a well-balanced nonlinear optical behavior5Structural diversity and photocurrent responses of multi-component chalcogenidometalates8Hetero‐Anionic Oxychalcogenides with Structures and Properties Tuned by the O:S Ratio14Photoluminescence-based temperature sensing in Nd³⁺-Doped tellurite glasses8Discovering Pseudo-Supertetrahedral Functional Units in Salt-Inclusion Nonlinear Optical Material [Ba22(SO4)5][Zn14Ga18S58]14Oxygen‐Substitution Induced High‐Performance Nonlinear Optical Properties: Witnessed by the First Quaternary Oxythiostannate12Zero-Dimensional Oxyselenide Ba12[(Ga2OSe5)3(Si2O7)]: Enhanced Optical Anisotropy through Heteroanionic Engineering4A Series of Pentanary Rare-Earth Oxysulfides Obtained by Heterovalent Cation and Anion Cosubstitution Exhibiting Nonlinear Optical Activity and Ultrawide Band Gaps1Eu(II) 4 Eu(III) 2 Ge 3 S 11 O 2 : a Single‐Element Mixed‐Valence Engineering Breakthrough for Strongly Enhanced Nonlinearity and Anisotropy in Rare‐Earth Oxysulfides8Synergistic Enhancement of Band Gap and Optical Anisotropy via Functional-Site Cosubstitution in Antiperovskite-Type Chalcohalides [Ba2K][X][MS4] (M = Ge, Si; X = Cl, Br)2A high-performance IR nonlinear optical material Sr 3 MnGe 2 S 8 achieved via partial cation substitution-induced structural transformation2Ba 3 S[SnOS 3 ] and [Ba 2 Sn]S[Ge 2 O 7 ]: two antiperovskite oxychalcogenides with good IR nonlinear optical performances2Strong Piezoelectric Response in an Oxalate-Coordinated Aluminum Crystal NaBaAl(C 2 O 4 ) 3 ·5H 2 O0Inorganic Ge-based ferroelectric perovskites towards quasi-phase-matching in the infrared region0From KBa 4 Ge 3 S 10 Cl to ABa 3 EuGe 3 S 11 (A = Na, K) Synthesized by Reactive Flux Assisted Metal Oxide-Boron-Chalcogen (MOBQ) Method: Effect of Cation/Anion Cosubstitution on Crystal Structure and Nonlinear Optical Properties0Heterometallic Ge–O–Sn-Bridged Oxychalcogenides Sr3GeSnO4Q3 (Q = S, Se) with Wide Band Gaps and Moderate Infrared Nonlinear Optical Responses0AVP2S7 (A = K, Rb): Dual-Optimized Infrared Nonlinear Optical Thiophosphates via Heterovalent-Substitution-Driven Symmetry Breaking and Reinforced Interlayer Interactions0AgEuPS4: Unlocking the Centrosymmetric Shackle of Rare-Earth Thiophosphates via Microscopic Distortion Cascading for Enhanced Second-Harmonic Generation Response0

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  1. 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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  2. An overview of Mg-based IR nonlinear optical materials

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  3. From CdPb 8 (SeO 3 ) 4 Br 10 to Pb 3 (TeO 3 )Br 4 : the first tellurite bromide exhibiting an SHG response and mid-IR transparency

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

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  5. Melilite oxychalcogenide Sr 2 FeGe 2 OS 6 : a phase-matching IR nonlinear optical material realized by isomorphous substitution

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  6. Stereochemically active lone-pair-driven giant enhancement of birefringence from three-dimensional CsZn 4 Ga 5 Se 12 to two-dimensional CsZnAsSe 3

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  7. Water‐Assisted Growth of Twisted 3R‐Stacked MoSe 2 Spirals and Its Dramatically Enhanced Second Harmonic Generations

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  8. Recent progress of newly developed functional building units and corresponding nonlinear optical materials

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  9. AAl(Te 4 O 10 ) (A = Na, Ag) and K 2 Ga 2 (HTe 6 O 16 )(HTeO 3 ): Three Aluminum/Gallium Tellurites with Large Birefringence and Wide Band Gap

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  10. Recent advances in IR nonlinear optical chalcogenides with well-balanced comprehensive performance

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  11. Cd2Nb2Te4O15: A Novel Pseudo‐Aurivillius‐Type Tellurite with Unprecedented Nonlinear Optical Properties and Excellent Stability

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  12. Three-in-One Tetrahedral Functional Units Constructing Diamondlike Ag2In2SiS3.06Se2.94 with High-Performance Nonlinear-Optical Activity

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  13. A survey of stereoactive oxysalts for linear and nonlinear optical applications

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  14. Four UV Transparent Linear and Nonlinear Optical Materials Explored from Pure Selenite Compounds

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  15. Breaking Through the Trade‐Off Between Wide Band Gap and Large SHG Coefficient in Mercury‐Based Chalcogenides for IR Nonlinear Optical Application

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  16. Chiral and Polar Duality Design of Heteroanionic Compounds: Sr18Ge9O5S31 Based on [Sr3OGeS3]2+ and [Sr3SGeS3]2+ Groups

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  17. Ga-based IR nonlinear optical materials: Synthesis, structures, and properties

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  18. “Three‐in‐One”: A New Hg‐Based Selenide Hg 7 P 2 Se 12 Exhibiting Wide Infrared Transparency Range and Strong Nonlinear Optical Effect

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  19. A UV non-hydrogen pure selenite nonlinear optical material for achieving balanced properties through framework-optimized structural transformation

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  20. Chemical modulation of A I RE III C IV QVI4 family compounds for band gap and optical anisotropy enhancement

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  21. Chemical perspectives on heteroanionic compounds: a potential playground for multiferroics

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  22. New nonlinear optical oxyfluoride K 2 NbO 2 F 3 with strong pseudo-centrosymmetry, obtained by mild hydrothermal synthesis

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  23. Partial 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)

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

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  25. RbPbPS 4 : a promising IR nonlinear optical material achieved by lone-pair-cation-substitution-induced structure transformation

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  26. Salt-inclusion sulfides [K 4 Cl][M II 11 In 9 S 26 ] (M II = Zn, Cd) displaying robust nonlinear optical activity

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  27. Hg3Se(SeO3)(SO4): A Mixed-Valent Selenium Compound with Mid-Infrared Transmittance Obtained by In Situ Reaction

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  28. KREP 2 S 6 (RE = Sm, Gd, Tb, Dy): A Series of Polar Rare-Earth Thiophosphates with High Laser-Induced Damage Thresholds and Moderate Nonlinear-Optical Responses Synergistically Contributed by Isolated P 2 S 6 Units and {[RE 2 S 15 ] 24– } ∞ Layers

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  30. Reduction of Germanium Oxides–The Mixed-Valence Germanates A2Ge4O7 (A = Na, K)

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  31. Hg4(Te2O5)(SO4): A Giant Birefringent Sulfate Crystal Triggered by a Highly Selective Cation

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  32. Anhydrous Aluminum Iodate: Strong Second Harmonic Generation Effect Contributed by Unbonded and Antibonding Orbitals

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  33. Pentanary Oxythiogermanates Ba3MGe3O2S8 (M = Ca, Zn) Featuring [Ge3O2S8]8– Trimers and {[MGe3O2S8]6–}∞ Chains: Structural Chemistry and Physical Properties

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  34. The first Hg-based oxychalcogenide Sr2HgGe2OS6: Achieving balanced IR nonlinear optical properties through synergistic cation and anion substitution

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  35. Polymorphism of Niobium Phosphate Bronze Na4Nb8P4O32Deduced by the Packings of Structural Units: A Centrosymmetric Phase

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  36. PbBeB2O5: A High-Performance Ultraviolet Nonlinear-Optical Crystal with Functional [BeB2O8]8– Group

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  38. Ag 2 GeS 3 : A Diamond‐Like Chalcogenide as an IR Nonlinear Optical Material with Outstanding Second‐Harmonic Generation Response

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  39. Realizing Excellent Infrared Nonlinear Optical Performance in Eu-Based Chalcogenides via Rational Cross Substitution Strategy

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  40. From [Ba3S][GeS4] to [Ba3CO3][MS4] (M = Ge, Sn): Enhancing optical anisotropy in IR birefringent crystals via functional group implantation

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  45. Exploring new horizons in mid-to-far infrared nonlinear optical crystals: the significant potential of trigonal pyramidal [TeS 3 ] 2− functional units

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  46. Isovalent cation substitution drives structural transformation and infrared nonlinear optical activity in Eu-based chalcogenides

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  49. Hetero‐Anionic Oxychalcogenides with Structures and Properties Tuned by the O:S Ratio

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  50. Photoluminescence-based temperature sensing in Nd³⁺-Doped tellurite glasses

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