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RESEARCH PAPER · Chemistry of Materials · 2021

LiB2O3F: A Beryllium-Free Deep-Ultraviolet Nonlinear Optical Material Designed Based on a Boron-Rich Strategy

Chun‐Li Hu, Jin Chen, Zhi Gang Fang, Ru‐Ling Tang, Jiang‐Gao Mao

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LiB2O3F: A Beryllium-Free Deep-Ultraviolet Nonlinear Optical Material Designed Based on a Boron-Rich StrategyOriginalA General Principle for DUV NLO Materials: π‐Conjugated Confinement Enlarges Band Gap**175A General Principle for DUV NLO Materials: π‐Conjugated Confinement Enlarges Band Gap**27Sr 3 B 14 O 24 : a new borate with a [B 14 O 30 ] fundamental building block and an unwonted 2D double layer11[C 3 N 6 H 7 ] 2 [B 3 O 3 F 4 (OH)]: a new hybrid birefringent crystal with strong optical anisotropy induced by mixed functional units85Li 3 [Al(PO 4 ) 2 (H 2 O) 1.5 ] and Na[AlP 2 O 7 ]: from 2D layered polar to 3D centrosymmetric framework structures8Sc 2 F 2 (B 2 O 5 ): a deep ultraviolet scandium borate fluoride exhibiting large birefringence induced by the synergistic effect of B 2 O 5 and ScO n F 2 groups38α-LiMB 9 O 15 (M = Sr, Pb): flexible [B 3 O 7 ] units leading to the low temperature phase of β-LiMB 9 O 15 (M = Sr, Pb)11Na 3 Ti 3 O 3 (SeO 3 ) 4 F: A Phase-Matchable Nonlinear-Optical Crystal with Enlarged Second-Harmonic-Generation Intensity and Band Gap20Toward the Rational Design of Mid‐Infrared Nonlinear Optical Materials with Targeted Properties via a Multi‐Level Data‐Driven Approach110Strong Nonlinearity Induced by Coaxial Alignment of Polar Chain and Dense [BO3] Units in CaZn2(BO3)212Strong Nonlinearity Induced by Coaxial Alignment of Polar Chain and Dense [BO3] Units in CaZn2(BO3)2212Uncovering the Structural Diversity and Excellent Performance of a Deep Ultraviolet Nonlinear Optical System Li(B2O3)nF (n= 1, 1.5, 2, and 3) by Multicomponent Prediction26The Combination of Structure Prediction and Experiment for the Exploration of Alkali‐Earth Metal‐Contained Chalcopyrite‐Like IR Nonlinear Optical Material104An Optimized KBe2BO3F2‐Like Structure: The Unity of Deep‐Ultraviolet Transparency, Nonlinear Optical Property, and Ferroelectricity22Enhancement of Birefringence in Borophosphate Pushing Phase-Matching into the Short-Wavelength Region150Deep-ultraviolet nonlinear optical crystals: concept development and materials discovery181Hg2P2S6: A layered mercury hexathiodiphosphate (IV) with large birefringence11Rearrangement of [B2O5] Dimers within [B7O14] Clusters Enables Enhanced Optical Anisotropy in Li3Cs6Al2B14O28F4A new birefringent material, HfF2(IO3)2, with a large birefringence and improved overall performances achieved by the integration of functional groups19Ag[SC(NH2)2]2F: A Laser Damage-Tolerant Infrared Nonlinear Optical Material9Achieving Large Second Harmonic Generation Effects via Optimal Planar Alignment of Triangular Units64Phonon structure engineering for intrinsically spectrally selective emitters by anion groups0Cs[B 3 O 3 F 2 (OH) 2 ]: discovery of a hydroxyfluorooxoborate guided by selective organic–inorganic transformation13LiCs 3 AlB 7 O 14 : achieving enhanced optical anisotropy via [AlO 4 ] tetrahedron introduction to rearrange the anionic framework5Three-dimensional porous borocarbonitride composed of pentagonal motifs as a high-performance pyroelectric material0Zn2BS3Br: An Infrared Nonlinear Optical Material with Significant Dual-Property Enhancements Designed through a Template Grafting Strategy20CaB2O2F4: A Novel [BOF2]∞-Based Structural Template with a Strong Second Harmonic Generation Response and Large Band Gap2Prediction of Promising Deep Ultraviolet Nonlinear Optical Materials in the Li 2 O–B 2 O 3 System7A survey of stereoactive oxysalts for linear and nonlinear optical applications40Deep-ultraviolet (DUV) nonlinear optical (NLO) crystals: An application in photonic technologies29Heterologous Isomorphic Substitution Induces Optical Property Enhancement for Deep-UV Crystals: a Case in Rb[B3O3F2(OH)2]10Breaking the Inherent Interarrangement of [B3O6] Clusters for Nonlinear Optics with Orbital Hybridization Enhancement142Hydroxyl-Driven Enhanced Birefringence in Borophosphates3Fluorination Strategy Towards Symmetry Breaking of Boron‐centered Tetrahedron for Poly‐fluorinated Optical Crystals15Fluorination Strategy Towards Symmetry Breaking of Boron‐centered Tetrahedron for Poly‐fluorinated Optical Crystals70Ca 3 Al 2 B 8 O 18 : borate with a graphene-like layer featuring two types of topological six-membered rings induced by [AlO 4 ] units7Discovery of excellent ultraviolet nonlinear optical materials in chlorates and bromates with highly stereochemically active lone pairs12Design of deep-ultraviolet zero-order waveplate materials using LiB3O5 as the template8Toward the ultraviolet (UV) or deep-UV nonlinear optical crystals: The combination of π-conjugated planar [XY3] and tetrahedral [XY4]80Extending Unique 1D Double-Chains to 2D Layers with Birefringent Gain by Introducing a Hydroxyl Group5LiNa2Ca8B12O24F6Cl and Li1.2Na2.8B6O11: A Case of Cation-Induced Birefringence Enhancement via Dimensional Changes of Highly Polymerized [B12O24] Motifs10Looking Back the Nonlinear Optical Crystals in a Functionalized Unit's Perspective109A new ultraviolet-transparent molybdate featuring a layered structure and moderate birefringence0CN 4 H 7 B 3 O 3 F 2 (OH) 2 : short-wave UV hydroxyfluorooxyborate crystals with large birefringence2KNa 2 Y 2 B 2 O 6 F 3 : a beryllium free deep-UV nonlinear optical crystal with well-balanced properties2Li 2 CeRbB 18 O 30 and Li 2 Cs 2 SrB 18 O 30 : promising low-birefringence materials for UV and deep UV zero-order waveplates4Theoretical design of 2D Pca 2 1 SiNOX (X = H, F, and Cl) phases: a new family of flexible wide bandgap semiconductors2Highly Polarizable Phosphorus‐Centered Tetrahedra and π‐Conjugated Carbon‐Centered Triangular Moieties Inducing Large Anisotropy and Short‐Wavelength Phase‐Matching23K2PbB5P3O17: A Mixed-Coordinated Borophosphate with Enhanced Birefringence Driven by the [B2O5] Unit5Review of KBe2BO3F2-like second-order nonlinear optical materials and their structure-performance relationships13[CON3H6BF4]: An Efficient Metal‐Free Borate with Optimized Birefringence Achieved by Structural Design Strategy15Finding a Novel Borate Ferroelectric with Random Domain Structures for Deep‐UV Quasi‐Phase‐Matching22Phonon Structure Engineering for Intrinsically Spectrally Selective Emitters by Anion Groups0Extending the Chemistry of Scheelite‐type Oxides with Borates7Extending the Chemistry of Scheelite‐type Oxides with Borates2CsB(OH) 4 (H 2 O) 2 and Na(NH 4 ) 2 B 10 O 16 OH(H 2 O): a hydroxylation modification strategy regulates the borate structures and optical properties0Confinement-assembled ultraviolet nonlinear optical crystal from pyridine-expanded π-systems with exhibiting strong SHG and birefringence18Regulating B‐O Arrangement Boosts Anisotropy in a Simple Rubidium Borate, Leading to a High‐Performance UV NLO Crystal0Deep-Ultraviolet Transparent Zr/Hf Fluorides with Second-Harmonic Generation Effects Induced by Alkali-Metal Modulation2Accelerating the Discovery of Deep-Ultraviolet Nonlinear Optical Materials by Combining Machine Learning Interatomic Potentials with First-Principles Calculations: A Case of LiB2O3F0A Pyrazinamide–Iodic Acid Cocrystal Exhibiting Strong Second Harmonic Generation for Nonlinear Optics0

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  1. A General Principle for DUV NLO Materials: π‐Conjugated Confinement Enlarges Band Gap**

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  2. A General Principle for DUV NLO Materials: π‐Conjugated Confinement Enlarges Band Gap**

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  3. Sr 3 B 14 O 24 : a new borate with a [B 14 O 30 ] fundamental building block and an unwonted 2D double layer

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  4. [C 3 N 6 H 7 ] 2 [B 3 O 3 F 4 (OH)]: a new hybrid birefringent crystal with strong optical anisotropy induced by mixed functional units

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  5. Li 3 [Al(PO 4 ) 2 (H 2 O) 1.5 ] and Na[AlP 2 O 7 ]: from 2D layered polar to 3D centrosymmetric framework structures

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  6. Sc 2 F 2 (B 2 O 5 ): a deep ultraviolet scandium borate fluoride exhibiting large birefringence induced by the synergistic effect of B 2 O 5 and ScO n F 2 groups

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    Ru‐Ling Tang, Wei Xu, Weijie Xie, Chun‐Li Hu

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  7. α-LiMB 9 O 15 (M = Sr, Pb): flexible [B 3 O 7 ] units leading to the low temperature phase of β-LiMB 9 O 15 (M = Sr, Pb)

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    Kaitong Liu, Jian Wei Han, Fuming Li, Shujuan Han, Zhihua Yang, Xuping Wang, Shilie Pan

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  8. Na 3 Ti 3 O 3 (SeO 3 ) 4 F: A Phase-Matchable Nonlinear-Optical Crystal with Enlarged Second-Harmonic-Generation Intensity and Band Gap

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  9. Toward the Rational Design of Mid‐Infrared Nonlinear Optical Materials with Targeted Properties via a Multi‐Level Data‐Driven Approach

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  10. Strong Nonlinearity Induced by Coaxial Alignment of Polar Chain and Dense [BO3] Units in CaZn2(BO3)2

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  11. Strong Nonlinearity Induced by Coaxial Alignment of Polar Chain and Dense [BO3] Units in CaZn2(BO3)2

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  12. Uncovering the Structural Diversity and Excellent Performance of a Deep Ultraviolet Nonlinear Optical System Li(B2O3)nF (n= 1, 1.5, 2, and 3) by Multicomponent Prediction

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  13. The Combination of Structure Prediction and Experiment for the Exploration of Alkali‐Earth Metal‐Contained Chalcopyrite‐Like IR Nonlinear Optical Material

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    Peng Wang, Yu Chu, Abudukadi Tudi, Congwei Xie, Zhihua Yang, Shilie Pan, Junjie Li

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  14. An Optimized KBe2BO3F2‐Like Structure: The Unity of Deep‐Ultraviolet Transparency, Nonlinear Optical Property, and Ferroelectricity

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

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

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  17. Hg2P2S6: A layered mercury hexathiodiphosphate (IV) with large birefringence

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  18. Rearrangement of [B2O5] Dimers within [B7O14] Clusters Enables Enhanced Optical Anisotropy in Li3Cs6Al2B14O28F

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  19. A new birefringent material, HfF2(IO3)2, with a large birefringence and improved overall performances achieved by the integration of functional groups

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  20. Ag[SC(NH2)2]2F: A Laser Damage-Tolerant Infrared Nonlinear Optical Material

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  21. Achieving Large Second Harmonic Generation Effects via Optimal Planar Alignment of Triangular Units

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  22. Phonon structure engineering for intrinsically spectrally selective emitters by anion groups

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  23. Cs[B 3 O 3 F 2 (OH) 2 ]: discovery of a hydroxyfluorooxoborate guided by selective organic–inorganic transformation

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  24. LiCs 3 AlB 7 O 14 : achieving enhanced optical anisotropy via [AlO 4 ] tetrahedron introduction to rearrange the anionic framework

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  25. Three-dimensional porous borocarbonitride composed of pentagonal motifs as a high-performance pyroelectric material

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  26. Zn2BS3Br: An Infrared Nonlinear Optical Material with Significant Dual-Property Enhancements Designed through a Template Grafting Strategy

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  27. CaB2O2F4: A Novel [BOF2]∞-Based Structural Template with a Strong Second Harmonic Generation Response and Large Band Gap

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  28. Prediction of Promising Deep Ultraviolet Nonlinear Optical Materials in the Li 2 O–B 2 O 3 System

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

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  30. Deep-ultraviolet (DUV) nonlinear optical (NLO) crystals: An application in photonic technologies

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  31. Heterologous Isomorphic Substitution Induces Optical Property Enhancement for Deep-UV Crystals: a Case in Rb[B3O3F2(OH)2]

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  32. Breaking the Inherent Interarrangement of [B3O6] Clusters for Nonlinear Optics with Orbital Hybridization Enhancement

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  33. Hydroxyl-Driven Enhanced Birefringence in Borophosphates

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  34. Fluorination Strategy Towards Symmetry Breaking of Boron‐centered Tetrahedron for Poly‐fluorinated Optical Crystals

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  35. Fluorination Strategy Towards Symmetry Breaking of Boron‐centered Tetrahedron for Poly‐fluorinated Optical Crystals

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  36. Ca 3 Al 2 B 8 O 18 : borate with a graphene-like layer featuring two types of topological six-membered rings induced by [AlO 4 ] units

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  37. Discovery of excellent ultraviolet nonlinear optical materials in chlorates and bromates with highly stereochemically active lone pairs

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  38. Design of deep-ultraviolet zero-order waveplate materials using LiB3O5 as the template

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

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  40. Extending Unique 1D Double-Chains to 2D Layers with Birefringent Gain by Introducing a Hydroxyl Group

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  41. LiNa2Ca8B12O24F6Cl and Li1.2Na2.8B6O11: A Case of Cation-Induced Birefringence Enhancement via Dimensional Changes of Highly Polymerized [B12O24] Motifs

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  42. Looking Back the Nonlinear Optical Crystals in a Functionalized Unit's Perspective

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  43. A new ultraviolet-transparent molybdate featuring a layered structure and moderate birefringence

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  44. CN 4 H 7 B 3 O 3 F 2 (OH) 2 : short-wave UV hydroxyfluorooxyborate crystals with large birefringence

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  45. KNa 2 Y 2 B 2 O 6 F 3 : a beryllium free deep-UV nonlinear optical crystal with well-balanced properties

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  46. Li 2 CeRbB 18 O 30 and Li 2 Cs 2 SrB 18 O 30 : promising low-birefringence materials for UV and deep UV zero-order waveplates

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  47. Theoretical design of 2D Pca 2 1 SiNOX (X = H, F, and Cl) phases: a new family of flexible wide bandgap semiconductors

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  48. Highly Polarizable Phosphorus‐Centered Tetrahedra and π‐Conjugated Carbon‐Centered Triangular Moieties Inducing Large Anisotropy and Short‐Wavelength Phase‐Matching

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  49. K2PbB5P3O17: A Mixed-Coordinated Borophosphate with Enhanced Birefringence Driven by the [B2O5] Unit

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  50. Review of KBe2BO3F2-like second-order nonlinear optical materials and their structure-performance relationships

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