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RESEARCH PAPER · Journal of the American Chemical Society · 2020

Realizing Deep-Ultraviolet Second Harmonic Generation by First-Principles-Guided Materials Exploration in Hydroxyborates

Pifu Gong, Lei Kang, Zheshuai Lin

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Realizing Deep-Ultraviolet Second Harmonic Generation by First-Principles-Guided Materials Exploration in HydroxyboratesOriginalAB 11 O 16 (OH) 2 (A = K and Cs): interpenetrating 2D layers with large birefringence7Predicting Berborite as Potential Deep-Ultraviolet Nonlinear Optical Crystal from First Principles29Nonlinear Optical Oxythiophosphate Approaching the Good Balance with Wide Ultraviolet Transparency, Strong Second Harmonic Effect, and Large Birefringence92Nonlinear Optical Oxythiophosphate Approaching the Good Balance with Wide Ultraviolet Transparency, Strong Second Harmonic Effect, and Large Birefringence13Ba 4 Ca(B 2 O 5 ) 2 F 2 : π-conjugation of B 2 O 5 in the planar pentagonal layer achieving large second harmonic generation of pyro -borate34Computationally assisted multistage design and prediction driving the discovery of deep-ultraviolet nonlinear optical materials41Deep-ultraviolet transparent alkali metal–rare earth metal sulfate NaY(SO 4 ) 2 ·H 2 O as a nonlinear optical crystal: synthesis and characterization28KB 3 H 8 : an environment-friendly reagent for the selective reduction of aldehydes and ketones to alcohols12M 6 PS 5 X (M = Ag, Cu; X = Cl, Br) chalcohalides exhibiting strong nonlinear optical responses and high laser damage resistances9Regulating Guanidinium-Based Hybrid Materials for Ultraviolet Nonlinear Optical Applications by Hybrid Strength and Hybrid Pattern26Prediction of Novel van der Waals Boron Oxides with Superior Deep‐Ultraviolet Nonlinear Optical Performance43Prediction of Novel van der Waals Boron Oxides with Superior Deep‐Ultraviolet Nonlinear Optical Performance6LiZn(OH)CO3: A Deep‐Ultraviolet Nonlinear Optical Hydroxycarbonate Designed from a Diamond‐like Structure180LiZn(OH)CO3: A Deep‐Ultraviolet Nonlinear Optical Hydroxycarbonate Designed from a Diamond‐like Structure10Deep‐Ultraviolet Nonlinear‐Optical van‐der‐Waals Beryllium Borates**6Exploring Deep-UV Nonlinear Optical Materials with Enhanced Second Harmonic Generation Response and Birefringence in Fluoroaluminoborate Crystals69Mg 2 In 3 Si 2 P 7 : A Quaternary Diamond-like Phosphide Infrared Nonlinear Optical Material Derived from ZnGeP 2130Novel van der Waals Deep‐UV Nonlinear Optical Materials32D van der Waals Layered [C(NH2)3]2SO3S Exhibits Desirable UV Nonlinear-Optical Trade-Off47Achieving Short‐Wavelength Phase‐Matching Second Harmonic Generation in Boron‐Rich Borosulfate with Planar [BO3] Units102Achieving Short‐Wavelength Phase‐Matching Second Harmonic Generation in Boron‐Rich Borosulfate with Planar [BO3] Units9Strong SHG Responses in a Beryllium‐Free Deep‐UV‐Transparent Hydroxyborate via Covalent Bond Modification89Strong SHG Responses in a Beryllium‐Free Deep‐UV‐Transparent Hydroxyborate via Covalent Bond Modification9A Potassium Tungsten Oxyfluoride with Strong Second-Harmonic Generation Response Derived from Anion-Ordered Functional Motif18Machine Learning with Multilevel Descriptors for Screening of Inorganic Nonlinear Optical Crystals35Ba2B13O19(OH)5·5H2O: A promising nonlinear optical material with a unique 2[B13O19(OH)5]∞ two-dimensional layer9A Lanthanum Ammonium Sulfate Double Salt with a Strong SHG Response and Wide Deep‐UV Transparency15A Lanthanum Ammonium Sulfate Double Salt with a Strong SHG Response and Wide Deep‐UV Transparency96KLi 2 CO 3 F: a beryllium-free KBBF-type deep-UV carbonate with an enhanced interlayer interaction and large birefringence20Nain(C2o4)(Hpo4)(H2o)5: An Ultraviolet Transparent Nonlinear Optical Oxalate-Phosphate with Large Birefringence0Performance of optical materials with the derivative of planar π-conjugated groups: Recent advances and future prospects37HgTeO2F(OH): A Nonlinear Optical Oxyfluoride Constructed of Active [TeO2F(OH)]2– Pyramids and V-Shaped [HgO2]2– Groups36Review of Heteroleptic Tetrahedra as Birefringent or Nonlinear Optical Motifs17Inorganic nonlinear optical materials7Ultrawide Bandgap and Outstanding Second‐Harmonic Generation Response by a Fluorine‐Enrichment Strategy at a Transition‐Metal Oxyfluoride Nonlinear Optical Material51Ultrawide Bandgap and Outstanding Second‐Harmonic Generation Response by a Fluorine‐Enrichment Strategy at a Transition‐Metal Oxyfluoride Nonlinear Optical Material12Alkali metal sulfate: A new non-π-conjugated deep-ultraviolet quasi-phase matching crystal27Promising Deep‐Ultraviolet Birefringent Materials via Rational Design and Assembly of Planar π‐Conjugated [B(OH)3] and [B3O3(OH)3] Functional Species6Promising Deep‐Ultraviolet Birefringent Materials via Rational Design and Assembly of Planar π‐Conjugated [B(OH)3] and [B3O3(OH)3] Functional Species83An 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 discovery181Design of a new ultraviolet nonlinear optical material KNO3SO3NH3 exhibiting an unexpected strong second harmonic generation response44Cs2B4O5(OH)4: A new hydrated borate with a short UV cutoff edge2Isoreticular Design of KTiOPO 4 -Like Deep-Ultraviolet Transparent Materials Exhibiting Strong Second-Harmonic Generation68CaBO2F: A novel deep-UV structural template with high nonlinear optical performance induced by electron delocalization25Role of large Rashba spin-orbit coupling in second-order nonlinear optical effects of polar BiB3O627Deep-ultraviolet nonlinear-optical crystal BaNa2[PO3(OH)]2 with large birefringence and strong second-harmonic-generation response8Recent progress in borate-based short-wavelength nonlinear optical crystals with boron–oxygen skeleton modification28Rational Design of the First Ammonium Magnesium Borate with Deep-Ultraviolet Cutoff Edge and Moderate Birefringence and Further Investigation into the Nature of Ammonium in the Borate System15“Cation Activation”: An Effective Strategy for the Enhancement of Birefringence36Target-Oriented Synthesis of Borate Derivatives Featuring Isolated [B3O3] Six-Membered Rings as Structural Features20Improved Birefringence Activated by Tetrahedra Decorated with a Single Linear Unit38Improved Birefringence Activated by Tetrahedra Decorated with a Single Linear Unit1Fluorooxoborate Promoting the Exploration of Short-Wavelength Linear and Nonlinear Optical Crystals with Expected Properties and Versatile Structures27Introduction of the [B–O/F] Units Enhances the Band Gap and Birefringence from Na6Mg3B10O18F6 to K3NaB10O16F211A Non‐π‐Conjugated Molecular Crystal with Balanced Second‐Harmonic Generation, Bandgap, and Birefringence10The synthesis of novel lanthanum hydroxyborate at extreme conditions3Enlargement 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 Region23Hydroxyl-Driven Enhanced Birefringence in Borophosphates3Achieving strong second harmonic generation effects induced via dimensional increase of PbX 6 octahedra and halogen substitutes in (C 10 H 11 N 3 )PbX 4 (X = Cl or Br)26Exploring a new short-wavelength nonlinear optical fluoride material featuring unprecedented polar cis -[Zr 6 F 34 ] 10− clusters48K, Rb-hydroxyborates series with deep-ultraviolet KRbB 5 O 8 (OH) possessing moderate second harmonic generation response0KBa 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 moieties37NaB(OH) 3 CH 3 : a deep-ultraviolet optical crystal with unprecedented methyl-modified [B(OH) 3 CH 3 ] units6Shooting short-wavelength nonlinear optical materials with targeted balance performances in hydroxyborates through first-principles high-throughput screening4Strategically designed metal-free deep-ultraviolet birefringent crystals with superior optical properties18Toward the ultraviolet (UV) or deep-UV nonlinear optical crystals: The combination of π-conjugated planar [XY3] and tetrahedral [XY4]80Boosted 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 Ligand48Unleashing the potential of π-conjugated [B2O3(OH)2] to enhance birefringence in DUV crystals9Extending Unique 1D Double-Chains to 2D Layers with Birefringent Gain by Introducing a Hydroxyl Group5Theoretical Understanding of Nonlinear Optical Properties in Solids: A Perspective27Edge-Sharing Tetrahedra Realizing Superior Birefringence and High Deep-Ultraviolet Transmittance in α-Be3(H2O)2(PO4)2 Crystal Synthesized by Mild Chemistry14NaRbB10O14(OH)4 and Na3CsB10O16(OH)2: Two Cases of Hydroxyborates with [B5Om(OH)n] Units and Deep Ultraviolet Cutoff Edges6Homoatomic Polychalcogenide Nonlinear Optical Anionic Groups with Ultra-Large Optical Anisotropy31Review on birefringence in borates based on birefringence-active functional groups and arrangements57Fluorine-driven materials design of novel deep-ultraviolet nonlinear optical crystal materials: Research progress and challenges6Exploiting Deep‐Ultraviolet Nonlinear Optical Material Rb 2 ScB 3 O 6 F 2 Originated from Congruously Oriented [B 3 O 6 ] Groups61Exploiting Deep‐Ultraviolet Nonlinear Optical Material Rb 2 ScB 3 O 6 F 2 Originated from Congruously Oriented [B 3 O 6 ] Groups4Lanthanide Contraction Eliminates Disorder while Holding Robust Second Harmonic Generation in a Series of Polyiodates13Structural Evolution and Optical Properties of Hydroxyfluorooxoborates MM′2n-1[B3O3F4(OH)]n (M = K, Cs, and Rb; M′ = K, NH4, and Cs; n = 1, 2, and 3)12Computer‐Aided Development of New Nonlinear Optical Materials38Computer‐Aided Development of New Nonlinear Optical Materials14Structural modification of hydroxyborates by adjusting the number of shared oxygen atoms and hydroxyl groups for further performance enhancement1Cation tuning in anionic framework hydroborates: tailored deep-ultraviolet optical crystals with large birefringence1CsBO(OH) 2 : a new hydroxyborate with the rare [BO(OH) 2 ] group and a deep ultraviolet cutoff edge3Pb 2 B 10 O 16 (OH) 2 ·B(OH) 3 ·H 2 O: significantly enhanced second harmonic generation via substituting metal cations in isostructural compounds with Pb 2+2RbB 7 O 10 (OH) 2 and NaB 11 O 16 (OH) 2 : alkali metal hydroxyborates with two-dimensional layered structures and large birefringence1层状结构深紫外非线性光学晶体研究进展（特邀）2Designing a 3‐Hydroxypropane‐1‐Sulfonate Deep‐Ultraviolet Nonlinear Optical Crystal9Non-equivalent terminating roles of hydroxyl and fluorine in hydroxy/fluorooxo-borate optical functional materials2NH4B5O7(OH)2 and CsRbB10O14(OH)4·H2O: Two Hydroxyborates Feature Significant Optical Anisotropy and Contain 1∞[B5O7(OH)2] Chains1Anion-Ordered [B3O5(OH)2] Induced by Crystal Water with Deep Ultraviolet Transparency and Large Birefringence in Boron-Rich Borophosphates4Na6(SO4)2SiF6: A Stable Sulfate Fluosilicate with Wide Deep-Ultraviolet Transparency Window and Strong Second-Harmonic Generation Response4Shape‐Topology‐Driven Design of Deep Ultraviolet Nonlinear Optical Crystals: Engineering [CH 3 PO 3 ]–Metal‐Oxo Layered Frameworks for Enhanced SHG, DUV Transparency3Hydroxyl-induced structural reconstruction: two new potassium hepta-borates with deep-UV transparency and enhanced birefringence1Synthesis, crystal structure and thermal behavior of Sr[B 8 O 11 (OH) 4 ] – synthetic analog of strontioborite0CsB(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 properties0孤对电子效应羟基硼酸盐非线性光学研究进展（特邀）0Ba 5 Zn 4 (B 3 O 6 ) 2 (B 12 O 24 ): A Borate with Edge-Sharing [BO 4 ] Tetrahedral Connection by Introducing Zn into β-BaB 2 O 42Confinement π‐Conjugated Moiety Tailoring to Achieve Record Deep‐UV Nonlinearity in Sulfates0The Enhancement of Phase‐Matching Capability by Recombining π‐Conjugated Group in Nonlinear Optical Sulfates1F−/OH− terminal modification of [B3O6] clusters: Constructing deep-ultraviolet hydroxyfluorooxoborates with tunable optical performance0Regulating B‐O Arrangement Boosts Anisotropy in a Simple Rubidium Borate, Leading to a High‐Performance UV NLO Crystal0K 3 Yb 2 (BO 3 ) 3 and Rb 3 Yb 2 (BO 3 ) 3 : Two Rare-Earth Borate Ultraviolet Nonlinear Optical Crystals1Toward the vacuum-ultraviolet frontier in nonlinear optical frequency conversion: phase-matching mechanisms across dimensions and architectures2From High Symmetry to High Symmetry: A Self‐Assembly Strategy for Synthesizing Large Birefringent Borates0Advances in metal selenite nonlinear optical materials: halogens directed structure modulation and property optimization0Cation‐Regulated [CH 3 BO 2 F]‐Derived Borates: Synergistic Fluorination and Organic Functionalization for High‐Birefringence UV NLO Materials0

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  2. Predicting Berborite as Potential Deep-Ultraviolet Nonlinear Optical Crystal from First Principles

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  3. Nonlinear Optical Oxythiophosphate Approaching the Good Balance with Wide Ultraviolet Transparency, Strong Second Harmonic Effect, and Large Birefringence

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  4. Nonlinear Optical Oxythiophosphate Approaching the Good Balance with Wide Ultraviolet Transparency, Strong Second Harmonic Effect, and Large Birefringence

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  5. Ba 4 Ca(B 2 O 5 ) 2 F 2 : π-conjugation of B 2 O 5 in the planar pentagonal layer achieving large second harmonic generation of pyro -borate

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  10. Regulating Guanidinium-Based Hybrid Materials for Ultraviolet Nonlinear Optical Applications by Hybrid Strength and Hybrid Pattern

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  12. Prediction of Novel van der Waals Boron Oxides with Superior Deep‐Ultraviolet Nonlinear Optical Performance

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  13. LiZn(OH)CO3: A Deep‐Ultraviolet Nonlinear Optical Hydroxycarbonate Designed from a Diamond‐like Structure

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  14. LiZn(OH)CO3: A Deep‐Ultraviolet Nonlinear Optical Hydroxycarbonate Designed from a Diamond‐like Structure

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  15. Deep‐Ultraviolet Nonlinear‐Optical van‐der‐Waals Beryllium Borates**

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  33. Review of Heteroleptic Tetrahedra as Birefringent or Nonlinear Optical Motifs

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  34. Inorganic nonlinear optical materials

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  35. Ultrawide Bandgap and Outstanding Second‐Harmonic Generation Response by a Fluorine‐Enrichment Strategy at a Transition‐Metal Oxyfluoride Nonlinear Optical Material

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  36. Ultrawide Bandgap and Outstanding Second‐Harmonic Generation Response by a Fluorine‐Enrichment Strategy at a Transition‐Metal Oxyfluoride Nonlinear Optical Material

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  37. Alkali metal sulfate: A new non-π-conjugated deep-ultraviolet quasi-phase matching crystal

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  38. Promising Deep‐Ultraviolet Birefringent Materials via Rational Design and Assembly of Planar π‐Conjugated [B(OH)3] and [B3O3(OH)3] Functional Species

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

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

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  43. Design of a new ultraviolet nonlinear optical material KNO3SO3NH3 exhibiting an unexpected strong second harmonic generation response

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  44. Cs2B4O5(OH)4: A new hydrated borate with a short UV cutoff edge

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  45. Isoreticular Design of KTiOPO 4 -Like Deep-Ultraviolet Transparent Materials Exhibiting Strong Second-Harmonic Generation

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  46. CaBO2F: A novel deep-UV structural template with high nonlinear optical performance induced by electron delocalization

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  47. Role of large Rashba spin-orbit coupling in second-order nonlinear optical effects of polar BiB3O6

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

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  49. Recent progress in borate-based short-wavelength nonlinear optical crystals with boron–oxygen skeleton modification

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