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RESEARCH PAPER · Chemistry of Materials · 2021

Recent Development of Non-π-Conjugated Deep Ultraviolet Nonlinear Optical Materials

Weiqi Huang, Sangen Zhao, Junhua Luo

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Recent Development of Non-π-Conjugated Deep Ultraviolet Nonlinear Optical MaterialsOriginal(N 2 H 6 )[HPO 3 F] 2 : maximizing the optical anisotropy of deep-ultraviolet fluorophosphates33Synergistic effect of 2 [V 2 P 2 O 14 ] ∞ layers and hydrogen bonds inducing large birefringence in M(VO) 2 (PO 4 ) 2 ·4H 2 O (M = Ca, Sr, Ba) systems4“Removing Center”─An Effective Structure Design Strategy for Nonlinear Optical Crystals37A crystalline photochromic metalloviologen compound with a chiral ligand: Synthetic strategy and SHG-photoswitching property1Enhancement of Birefringence in Borophosphate Pushing Phase-Matching into the Short-Wavelength Region150Deep-ultraviolet nonlinear optical crystals: concept development and materials discovery181[C(NH2)3]2MoO2F4·H2O: Unique Chinese-Knot Structure Revealing Superior Nonlinear-Optical Properties19Oxychalcogenides as Promising Ultraviolet Nonlinear Optical Candidates: Experimental and Theoretical Studies of AEGeOS2(AE = Sr and Ba)24Design of novel deep-UV nonlinear optical materials with one-dimensional functional module [BO2]∞ chain and fluorine-driven short phase-matching43A High‐Performance Nonlinear Optical Crystal with a Building Block Containing Expanded π‐Delocalization95A High‐Performance Nonlinear Optical Crystal with a Building Block Containing Expanded π‐Delocalization5Local Polarity-Induced Assembly of Second-Order Nonlinear Optical Materials128Ba5Ga2SiO4S6: a Phase-Matching Nonlinear Optical Oxychalcogenide Design via Structural Regulation Originated from Heteroanion Introduction25A lithium–scandium sulfate with second-harmonic generation response and deep-ultraviolet transparency7Accurate design and synthesis of nonlinear optical crystals employing KBe2BO3F2 as structural template55An overview of Mg-based IR nonlinear optical materials22Anisotropic structure building unit involving diverse chemical bonds: a new opportunity for high-performance second-order NLO materials181Deep-ultraviolet nonlinear-optical crystal BaNa2[PO3(OH)]2 with large birefringence and strong second-harmonic-generation response8Modulating optical performance by phase transition in a nonlinear optical material β-Li 2 RbBi(PO 4 ) 28Nitrides: a promising class of nonlinear optical material candidates9Solvent-free synthesis of magnesium phosphite-oxalates that show second-harmonic generation responses5BaB2P2O8F2: A Fluoroborophosphate with [B2P2O8F2]∞ Layers and Deep-Ultraviolet Cutoff Edge4Machine Learning Regression Model for Predicting the Formation Energy of Nonlinear Optical Crystals5Recent advances of inorganic phosphates with UV/DUV cutoff edge and large second harmonic response7Recent advances in non-π-conjugated nonlinear optical sulfates with deep-UV absorption edge53Host–Guest Symmetry Matching in Two Crystalline Magnesium Sulfate Oxalates Obtained Via a Solvent-Free Route8Host–Guest Symmetry and Charge Matching in Glycine-Templated Metal Sulfate–Oxalates Obtained by a Solvent-Free Method9Recent advances in IR nonlinear optical chalcogenides with well-balanced comprehensive performance56Nonlinear optical inorganic sulfates: The improvement of the phase matching ability driven by the structural modulation41Quadruple‐Bidentate Nitrate‐Ligated A 2 Hg(NO 3 ) 4 (A=K, Rb): Strong Second‐Harmonic Generation and Sufficient Birefringence59Quadruple‐Bidentate Nitrate‐Ligated A 2 Hg(NO 3 ) 4 (A=K, Rb): Strong Second‐Harmonic Generation and Sufficient Birefringence2Li2RbSO4Cl with a Short Ultraviolet Absorption Edge and an Acentric Structure through Assembling Heteroleptic [LiO3Cl] Tetrahedra2Strategy for a Rational Design of Deep-Ultraviolet Nonlinear Optical Materials from Zeolites2Sr(NO 3 )(NH 2 SO 3 )·H 2 O: First Nitrate Sulfamate Revealing Remarkable Second Harmonic Generation and Optimized Birefringence25Enlargement of Bandgap and Birefringence in Nonlinear Optical Alkali‐Metal Sulfate Crystals by the Substitution of Asymmetrical Non‐π‐Conjugated Cation8(SO3CF3)−: A Non‐π‐Conjugated Motif for Nonlinear Optical Crystals Transparent into the Deep‐Ultraviolet Region23Deep‐Ultraviolet Transparent Mixed Metal Sulfamates with Enhanced Nonlinear Optical Properties and Birefringence11Deep‐Ultraviolet Transparent Mixed Metal Sulfamates with Enhanced Nonlinear Optical Properties and Birefringence75Hydroxyl-Driven Enhanced Birefringence in Borophosphates3The structural origin and boundaries of thermal transitions in stillwellite-type LnBSiO54Advances in Solid-State Nonlinear Optical Materials: From Fundamentals to Applications61Enhanced near-infrared optical transmission in zinc germanium phosphide crystals via precise magnesium doping3Exploring a new short-wavelength nonlinear optical fluoride material featuring unprecedented polar cis -[Zr 6 F 34 ] 10− clusters48Form-controlled synthesis of a polymorphic nonlinear optical crystal CsMgPO 4 ·6H 2 O3KBa 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 moieties37Optimized arrangement of non-π-conjugated PO 3 NH 3 units leads to enhanced ultraviolet optical nonlinearity in NaPO 3 NH 328新型深紫外非线性光学晶体研究进展（特邀）9Toward the ultraviolet (UV) or deep-UV nonlinear optical crystals: The combination of π-conjugated planar [XY3] and tetrahedral [XY4]80C(NH2)3MoO3(IO3): A Molybdenyl Iodate with Giant Birefringence Designed via a Cation–Anion Synergetic Interaction Strategy36Metal Methanesulfonates with Mixed Anionic Groups with Large Band Gaps and Enhanced Birefringence50Combining rigid and deformable groups to construct a robust birefringent crystal for compact polarization components25Assembly 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, Cs2YB3O6F297A Chlorinated Indolium‐Based Nonlinear Optical Crystal Achieving Effective Terahertz‐Wave Generation and Highly Sensitive Detection19Recent advances and future perspectives on rare-earth-based nonlinear optical materials with π-conjugated [XO3] (X = B, C, N) units66A3Sc(SO4)3 (A = K, Rb, Cs): Three Deep‐Ultraviolet Transparent Alkali‐Scandium Sulfates with Strong Second‐Harmonic Generation Response and High Thermal Stability14Advancements in Nonlinear Optical Materials: Paving the Way for Future Photonic Devices4Synthesis and Large Crystal Growth of a Noncentrosymmetric Sodium Methylsulfanetriol Borate Lewis-Adduct: Na(S(OH)3CH3)(BO3)10Achieving the Birefringence Optimization by Methyl Modulation in Organic Nonlinear Optical Crystals15Structure and optical properties of alkali rare-earth double phosphates of M3RE(PO4)2 (M = K, Rb; RE = Y, La, and Lu)4MgPO2F3: An Ultraviolet Nonlinear Optical System with an Extremely Short Phase-Matching Wavelength Achieved by Introducing Dual-Type Fluorine via Structure Prediction1Functional assembly and modification of nonlinear optical fundamental motifs in phosphates27The New Paradigm of Ligand Substitution-Driven Enhancement of Anisotropy from SO4 Units in Short-Wavelength Region14Spectroscopic studies and Non-Linear optical response through C/N replacement and modulation of electron Donor/Acceptor Units on naphthyridine derivatives24Looking Back the Nonlinear Optical Crystals in a Functionalized Unit's Perspective109Li3[AlP2O7F(OH)](H2O)0.5 and A[Al2(PO4)2F(H2O)](A = K, Rb): Counter Cation Templates Derived Three Polar Alkaline Metal Fluoroaluminophosphates6Cationic Coordination Modification Drives Birefringence and Nonlinear Effect Double Lifting in Sulfate4A remarkable solar-blind ultraviolet nonlinear optical crystal with comprehensive performance and enhanced thermal stability4A tri-alkali/alkaline-earth metal fluorophosphate deep-ultraviolet birefringent crystal with coexisting PO 3 F and PO 2 F 24An excellent ultraviolet nonlinear optical crystal derived from the polar methylphosphonate unit8Different p-block elements induce C 3 [111] octahedral distortion in titanium to generate an intense nonlinear effect14层状结构深紫外非线性光学晶体研究进展（特邀）2Highly Polarizable Phosphorus‐Centered Tetrahedra and π‐Conjugated Carbon‐Centered Triangular Moieties Inducing Large Anisotropy and Short‐Wavelength Phase‐Matching23Chiral-Unit-Oriented Design of Non-π-Conjugated Noncentrosymmetric Phosphates with Short Absorption Edges4K2PbB5P3O17: A Mixed-Coordinated Borophosphate with Enhanced Birefringence Driven by the [B2O5] Unit5Phase-Matching Second-Harmonic Generation in Zero-Dimensional Zinc Thiocyanates Ligated with Chiral Amino Acids6NH4PO3HCH3 and NH4PO3CH2NH3: Two Phosphate Derivatives with Deep-UV Cutoff Edges and Moderate Birefringence1Recent progress in structural design strategies of high-birefringence optical crystals54Lattice activation for air deposition of micrometer-grain Pb-Sn perovskite film realizing efficient and stable ideal-bandgap solar cells5Non-equivalent terminating roles of hydroxyl and fluorine in hydroxy/fluorooxo-borate optical functional materials2Designing High-Performance Short-Wave UV Tellurium-Based Mixed Halides Birefringent Crystals via Halogen Substitution Engineering4Hybrid Bismuth Halide with Rich Polymorphism and Second Harmonic Generation Response8Borosilicates as deep-ultraviolet transparent nonlinear optical crystals: Structural motifs, performance limits and future directions9Structure-property relationships in IR nonlinear optical chalcogenides with stereochemically active lone pairs29Ag(Te2O3)(PO4): The first Ag-containing phosphate-tellurite nonlinear optical crystal featuring novel zigzag layered structure0Design and Synthesis of a Rare Earth Borate Ultraviolet Nonlinear Optical Crystal K 3 Lu 2 (BO 3 ) 38π-Conjugated unit bridge for giant second-harmonic generation and birefringence in hybrid materials with dual heteroleptic polyhedra5Stepwise Substitution Strategy for Beryllium-Based Selenites with Enhanced SHG Response, Moderate Birefringence, and Short UV Cutoff Edges6Achieving record birefringence in metal-free semiorganic sulfate crystals via tetrahedral anionic group substitution0立体化学活性孤对电子与极性基元协同构筑高性能紫外非线性光学晶体（NH4）2Sb3F9SeO4（特邀）0Zn 4 (BO 3 ) 2 (CO 2 CH 2 NH 2 ) 2 ·H 2 O: An Organic–Inorganic Hybridized KBe 2 BO 3 F 2 -like Ultraviolet Nonlinear Optical Crystal3Sn 4+ /Sn 2+ Aliovalent Substitution: A Strategy for Local Structure Engineering to Enhance Birefringence and Trigger Structural Symmetry Transition0An UV Transparent Metal‐Free Sulfate With Giant Birefringence Enabled by Optimal Structural Anisotropy4Enhanced tripling-performance in [C(NH2)3]4P2O7·H2O as UV nonlinear optical material due to π-conjugated cation and hydrogen bonding intervention1{[Ge 2 S 7 ] 6– } ∞ Chains-Mediated Framework Reorganization Triggers Dimensional Upgrade and Infrared Nonlinear Optical Response3Accelerating the discovery of athermal deep-ultraviolet nonlinear optical crystals via physics-informed herarchical graph learning1Strong Optical Nonlinearity in Polar Hypophosphites via Chiral Cation Assembly1K 2 ZrSi 2 O 7 with a Wide Transmission Range and Enhanced Birefringence Induced by the d 0 -TM Zr-Based Units2Deep-Ultraviolet Transparent Zr/Hf Fluorides with Second-Harmonic Generation Effects Induced by Alkali-Metal Modulation2When Octahedra Learn to Be Prisms: Unlocking a Record Deep‑UV NLO Crystal0When Octahedra Learn to Be Prisms: Unlocking a Record Deep‑UV NLO Crystal0A Rare-Earth Borophosphate Ultraviolet Nonlinear Optical Crystal Featuring P–O–P Linkages0Efficient Broad-Power-Range Nonlinear Ultraviolet Emission via Endothermic Triplet–Triplet Annihilation Upconversion0Urea revisited: Isopropyl substitution for a balanced nonlinear optical performance0Two Rare Earth-Based Sulfates with Enhanced Birefringence and Broad Optical Transparency Window0Borophosphate-based second-order nonlinear optical materials: Advances in structural diversity and optical performance0

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  1. (N 2 H 6 )[HPO 3 F] 2 : maximizing the optical anisotropy of deep-ultraviolet fluorophosphates

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  3. “Removing Center”─An Effective Structure Design Strategy for Nonlinear Optical Crystals

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  4. A crystalline photochromic metalloviologen compound with a chiral ligand: Synthetic strategy and SHG-photoswitching property

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  5. Enhancement of Birefringence in Borophosphate Pushing Phase-Matching into the Short-Wavelength Region

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  6. Deep-ultraviolet nonlinear optical crystals: concept development and materials discovery

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  7. [C(NH2)3]2MoO2F4·H2O: Unique Chinese-Knot Structure Revealing Superior Nonlinear-Optical Properties

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  8. Oxychalcogenides as Promising Ultraviolet Nonlinear Optical Candidates: Experimental and Theoretical Studies of AEGeOS2(AE = Sr and Ba)

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  9. Design of novel deep-UV nonlinear optical materials with one-dimensional functional module [BO2]∞ chain and fluorine-driven short phase-matching

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  10. A High‐Performance Nonlinear Optical Crystal with a Building Block Containing Expanded π‐Delocalization

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  11. A High‐Performance Nonlinear Optical Crystal with a Building Block Containing Expanded π‐Delocalization

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  12. Local Polarity-Induced Assembly of Second-Order Nonlinear Optical Materials

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  13. Ba5Ga2SiO4S6: a Phase-Matching Nonlinear Optical Oxychalcogenide Design via Structural Regulation Originated from Heteroanion Introduction

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  14. A lithium–scandium sulfate with second-harmonic generation response and deep-ultraviolet transparency

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  15. Accurate design and synthesis of nonlinear optical crystals employing KBe2BO3F2 as structural template

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

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

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  18. Deep-ultraviolet nonlinear-optical crystal BaNa2[PO3(OH)]2 with large birefringence and strong second-harmonic-generation response

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  21. Solvent-free synthesis of magnesium phosphite-oxalates that show second-harmonic generation responses

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  27. Host–Guest Symmetry and Charge Matching in Glycine-Templated Metal Sulfate–Oxalates Obtained by a Solvent-Free Method

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  33. Strategy for a Rational Design of Deep-Ultraviolet Nonlinear Optical Materials from Zeolites

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  35. Enlargement of Bandgap and Birefringence in Nonlinear Optical Alkali‐Metal Sulfate Crystals by the Substitution of Asymmetrical Non‐π‐Conjugated Cation

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  36. (SO3CF3)−: A Non‐π‐Conjugated Motif for Nonlinear Optical Crystals Transparent into the Deep‐Ultraviolet Region

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  37. Deep‐Ultraviolet Transparent Mixed Metal Sulfamates with Enhanced Nonlinear Optical Properties and Birefringence

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  39. Hydroxyl-Driven Enhanced Birefringence in Borophosphates

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  40. The structural origin and boundaries of thermal transitions in stillwellite-type LnBSiO5

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  42. Enhanced near-infrared optical transmission in zinc germanium phosphide crystals via precise magnesium doping

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  43. Exploring a new short-wavelength nonlinear optical fluoride material featuring unprecedented polar cis -[Zr 6 F 34 ] 10− clusters

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  44. Form-controlled synthesis of a polymorphic nonlinear optical crystal CsMgPO 4 ·6H 2 O

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  46. Optimized arrangement of non-π-conjugated PO 3 NH 3 units leads to enhanced ultraviolet optical nonlinearity in NaPO 3 NH 3

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  47. 新型深紫外非线性光学晶体研究进展（特邀）

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  48. Toward the ultraviolet (UV) or deep-UV nonlinear optical crystals: The combination of π-conjugated planar [XY3] and tetrahedral [XY4]

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  49. C(NH2)3MoO3(IO3): A Molybdenyl Iodate with Giant Birefringence Designed via a Cation–Anion Synergetic Interaction Strategy

    Chemistry of Materials · 2024-02-08

    Wei Zeng, Yao Tian, Xuehua Dong, Ling Huang, Hongmei Zeng, Zhien Lin, Guohong Zou

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  50. Metal Methanesulfonates with Mixed Anionic Groups with Large Band Gaps and Enhanced Birefringence

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