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RESEARCH PAPER · Advanced Functional Materials · 2023

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

Yu Chu, Hongshan Wang, Quan Chen, Xin Su, Zuxin Chen, Zhihua Yang, Junjie Li, Shilie Pan

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“Three‐in‐One”: A New Hg‐Based Selenide Hg 7 P 2 Se 12 Exhibiting Wide Infrared Transparency Range and Strong Nonlinear Optical EffectOriginalChemical modulation of A I RE III C IV QVI4 family compounds for band gap and optical anisotropy enhancement16Heteroanionic [VO x S 4− x ] groups: tetrahedral units with large birefringence for mid-infrared nonlinear optical crystals9Pb 3.5 GeS 4 Br 3 : the first phase-matching thiogermanate halide infrared nonlinear optical material12Pb 6 Ba 3 Si 2 S 8 I 10 : a new thiohalide with a quasi-two-dimensional structure and wide band gap2Wide band gap selenide infrared nonlinear optical materials A II Mg 6 Ga 6 Se 16 with strong SHG responses and high laser-induced damage thresholds31β -CsHg 2 I 5 , a compound with rare [Hg 2 I 5 ] dimers and large optical anisotropy2A Chlorinated Indolium‐Based Nonlinear Optical Crystal Achieving Effective Terahertz‐Wave Generation and Highly Sensitive Detection19Sulfate Derivatives with Heteroleptic Tetrahedra: New Deep‐Ultraviolet Birefringent Materials in which Weak Interactions Modulate Functional Module Ordering61Sulfate Derivatives with Heteroleptic Tetrahedra: New Deep‐Ultraviolet Birefringent Materials in which Weak Interactions Modulate Functional Module Ordering4Constructing Ultraviolet Nonlinear Optical Crystals with Superior Thermal Stability Based on Organic π-Conjugated [HCOO] Groups6Achieving Phase‐Matching in Nonlinear Optical Materials CsM 2 In 2 S 6 (M = Cd/In, Hg/In) by the Incorporation of Unprecedented Trigonal Planar MS 3 Motifs6Computer‐Aided Development of New Nonlinear Optical Materials38Computer‐Aided Development of New Nonlinear Optical Materials14Hg4InS2Cl5: Achieving Giant Optical Anisotropy by Introducing Well‐Aligned Linear [Hg2S2] Units14Rare‐Earth Substitution Induced Symmetry Breaking for The First Sc‐Based Nonlinear Optical Chalcogenide with High‐Performance30“Three functions in one”: multifunctional rare-earth cyamelurates with magnetism, luminescence, and giant optical nonlinearity6(CN 4 H 7 ) 2 SO 4 ·H 2 O: high-performance metal-free ultraviolet birefringent crystal with KBBF-like configuration5A wide band gap selenohalide Cs 9 Si 8 Se 20 Cl with unprecedented [CsSe 7 Cl] mixed anionic units2BaSbBS 4 : a record-high-performance birefringent crystal identified by a target-driven closed-loop strategy28Cd 5 Te 4 O 12 X 2 (X = Cl, Br, I): a new oxyhalide family with [CdO 4 X] mixed anionic units and adjustable optical properties4Enhanced second-harmonic generation response in a chiral lead iodide induced by amino acid coordination8Exploring new horizons in mid-to-far infrared nonlinear optical crystals: the significant potential of trigonal pyramidal [TeS 3 ] 2− functional units18M 3 MoO 4 (HCO 3 ) (M = Rb and Cs): cation-tuned synthesis of two noncentrosymmetric molybdate-carbonates with isolated [MoO 4 ] and [HCO 3 ] groups0Non-centrosymmetric structures designed rationally via a “dimensionality addition” strategy toward the promising nonlinear optical family [A–X][In–Se] (A = K/Ba and Rb/Ba; X = Cl and Br)13Prismatic crystal field stabilized divalent rare-earth chalcogenide REIIBII6CIII6QVI16 with bifunctionality30Structural diversity and photocurrent responses of multi-component chalcogenidometalates8Hetero‐Anionic Oxychalcogenides with Structures and Properties Tuned by the O:S Ratio14AI2Mg3Ga12S22 (AI = K, Rb): T2-type supertetrahedra coupled with [MgS6] octahedra for designing wide-band gap infrared nonlinear optical materials with well-balanced properties16First-Principles High-Throughput Screening and Experimental Verification of III-VIB Transition Metal Chalcogenides Nonlinear Optical Crystals15Pb 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 Birefringence3Accelerating Discovery of Infrared Nonlinear Optical Materials with High Lattice Thermal Conductivity: Combining Machine Learning and First‐Principles Calculations10New Ways to Discover Novel Nonlinear Optical Materials: Scaling Machine Learning with Chemical Descriptors Information20Reinforced 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 116A new selenide semiconductor NaMn3Ga3Se8 with strong second-harmonic generation and significant luminescence property5Synergically Assembling Advantageous Groups toward High‐Performance Infrared Nonlinear Optical Materials A II CdSiSe 4 (A II = Sr, Ba)40SrZnGeSe 4 : a promising infrared nonlinear optical material with strong second harmonic generation and high laser-induced damage threshold4Synergistic Machine Learning Guided Discovery of ABa 3 (BSe 3 ) 2 X (A = Rb, Cs; X = Cl, Br, I): A Promising Family as Property‐Balanced IR Functional Materials10Planar [HgCl 3 ] and V‑Shaped [HgCl 2 ] Units Synergistically Creating a Prominent Halide Birefringent Crystal β ‐CsHg 2 Cl 5 with Wide‐Spectrum7The Influence of Different Group Distortions on the Structure–Property Relationship of Alkali Metal Thiophosphate0[TeSeS 2 ] 2− : The First Heterotriple‐Chalcogenide Motifs Decode Giant Mid‐Far Infrared Birefringence18[TeSeS 2 ] 2− : The First Heterotriple‐Chalcogenide Motifs Decode Giant Mid‐Far Infrared Birefringence4Cd 7 I 12 Q·As 4 Q n (Q = S, Se; n = 3, 4): In Situ Alteration of Functional Molecules in Polar Metal Inorganic Framework Tailoring High‐Performance Infrared Nonlinear Optical Crystals9Large Nonlinear Optical Response and Slowed Electron‐Phonon Scattering in a Kagome‐type Flat Band Semiconductor0Water Molecule-Driven Structural Evolution from Na2ZnCl4 to Na2ZnCl4·3H2O: A Route to Promising Deep-UV Nonlinear Optical Crystals0From Centrosymmetric Ca3Ge2O3S4 to Noncentrosymmetric Ca3Ge2O4Se3: A Nonlinear Optical Ca-Based Oxyselenide5Eu(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 Oxysulfides8Vacancy-driven tetrahedral distortion leading to exceptional second harmonic generation3[HgX 2 ] Linear Group Enabled Ultraviolet Birefringent Crystal RbHg 5 Br 11 with Strong Optical Anisotropy and Wide Bandgap12Modulating 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 Performance3NaAg3Ga8S14: A new diamond-like framework infrared nonlinear optical material derived from AgGaS26Reactive flux assisted metal oxide–boron–sulfur routine for syntheses of CsRESiS 4 (RE = Sm, Gd–Ho): featuring nonlinear optical activity and wide band gaps5Tuning birefringence in alkaline-earth metal oxyhalides through diverse mixed-cation coordination architectures1A mercury-based selenite with wide bandgap and moderate birefringence via cation substitution and partial fluorination1LiPb3GeS4Br3：含孤对电子功能化超四面体的红外非线性光学晶体（特邀）0Te–Se replacement induced structural transition and enhanced band gaps in Cd 5 Se 4 O 12 Cl 2 and Cd 5 Se 4 O 12 Br 21Zn 0.7 Hg 0.3 Ga 2 Se 4 : a defect diamond-like selenide with a balanced band gap and nonlinear optical response0Realizing Phase‐Matching of Nonlinear Optical [ABa 3 Br 2 ][Ga 5 Se 10 ] (A = Cs, Rb, K, Na) Through Large Anisotropic Lattice Distortion6Realizing Phase‐Matching of Nonlinear Optical [ABa 3 Br 2 ][Ga 5 Se 10 ] (A = Cs, Rb, K, Na) Through Large Anisotropic Lattice Distortion11A Multi-Scale Cross-Band Defense System Integrating Decoupled Visible, Dynamic Infrared Camouflage and Electromagnetic Shielding31Harnessing tetrahedral diversity: The path to superior diamond-like IR NLO crystals13Topology-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 Threshold22Strategic Integration Between Trigonal Architecture Construction and Molecular Polarization Enhancement for Record SHG Effect in Selenates4Strategic Integration Between Trigonal Architecture Construction and Molecular Polarization Enhancement for Record SHG Effect in Selenates0Ba 4 CdGa 2 S 6 F 4 : A Chalcohalide Birefringent Crystal with Large Band Gap Designed by the Cation and Anion Cosubstitution Strategy2KNa2(Hf,Zr)F7 and KNa2HfF7: isostructural fluorides with phase-matchable second-harmonic generation0Advancing flexible sensing systems: Deep learning-driven insights and future perspectives0Steric hindrance and hydrogen-bond networks synergistically directing molecular alignment for high-performance ultraviolet birefringent1Linear [ICl 2 ] Units Induced Giant Optical Anisotropy in AICl 2 (A = NH 4 , Rb): A Pathway to Advanced Birefringent Materials4Bridging Motifs Induced Ordered Arrangement Contributing Large Birefringence for Hg 4 BiQ 2 Cl 5 (Q═S, Se)1Gravity‐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 Prospects0Mineral‐Inspired and Computation‐Assisted Rational Design of Polar Gittinsite‐Type Thiophosphates With Exceptional Nonlinear Optical Performance3Cation-substitution-driven electronic, nonlinear optical, elastic, and thermal transport properties of layered AeHgGeSe4 (Ae = Ba, Sr): A first-principles study0AgEuPS4: Unlocking the Centrosymmetric Shackle of Rare-Earth Thiophosphates via Microscopic Distortion Cascading for Enhanced Second-Harmonic Generation Response0From AgGaSe2 to MIIGa2Se4 (MII = Zn, Cd): Heterovalent Substitution Creates Ordered Vacancies for Balanced IR-NLO Performance0AlGaS3: a wide band gap ternary diamond-like infrared nonlinear optical material with high laser-induced damage threshold1

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

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  2. Heteroanionic [VO x S 4− x ] groups: tetrahedral units with large birefringence for mid-infrared nonlinear optical crystals

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  3. Pb 3.5 GeS 4 Br 3 : the first phase-matching thiogermanate halide infrared nonlinear optical material

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  4. Pb 6 Ba 3 Si 2 S 8 I 10 : a new thiohalide with a quasi-two-dimensional structure and wide band gap

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  5. Wide band gap selenide infrared nonlinear optical materials A II Mg 6 Ga 6 Se 16 with strong SHG responses and high laser-induced damage thresholds

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  6. β -CsHg 2 I 5 , a compound with rare [Hg 2 I 5 ] dimers and large optical anisotropy

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  10. Constructing Ultraviolet Nonlinear Optical Crystals with Superior Thermal Stability Based on Organic π-Conjugated [HCOO] Groups

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  11. Achieving Phase‐Matching in Nonlinear Optical Materials CsM 2 In 2 S 6 (M = Cd/In, Hg/In) by the Incorporation of Unprecedented Trigonal Planar MS 3 Motifs

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  14. Hg4InS2Cl5: Achieving Giant Optical Anisotropy by Introducing Well‐Aligned Linear [Hg2S2] Units

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  15. Rare‐Earth Substitution Induced Symmetry Breaking for The First Sc‐Based Nonlinear Optical Chalcogenide with High‐Performance

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  16. “Three functions in one”: multifunctional rare-earth cyamelurates with magnetism, luminescence, and giant optical nonlinearity

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  17. (CN 4 H 7 ) 2 SO 4 ·H 2 O: high-performance metal-free ultraviolet birefringent crystal with KBBF-like configuration

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  18. A wide band gap selenohalide Cs 9 Si 8 Se 20 Cl with unprecedented [CsSe 7 Cl] mixed anionic units

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  19. BaSbBS 4 : a record-high-performance birefringent crystal identified by a target-driven closed-loop strategy

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  20. Cd 5 Te 4 O 12 X 2 (X = Cl, Br, I): a new oxyhalide family with [CdO 4 X] mixed anionic units and adjustable optical properties

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  21. Enhanced second-harmonic generation response in a chiral lead iodide induced by amino acid coordination

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  43. Cd 7 I 12 Q·As 4 Q n (Q = S, Se; n = 3, 4): In Situ Alteration of Functional Molecules in Polar Metal Inorganic Framework Tailoring High‐Performance Infrared Nonlinear Optical Crystals

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  46. From Centrosymmetric Ca3Ge2O3S4 to Noncentrosymmetric Ca3Ge2O4Se3: A Nonlinear Optical Ca-Based Oxyselenide

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  48. Vacancy-driven tetrahedral distortion leading to exceptional second harmonic generation

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  49. [HgX 2 ] Linear Group Enabled Ultraviolet Birefringent Crystal RbHg 5 Br 11 with Strong Optical Anisotropy and Wide Bandgap

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  50. Modulating Nonlinear Optical Performances in α/β-SnGa2GeS6 Polymorphs via Atomic Coordination Engineering

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