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RESEARCH PAPER · Journal of the American Chemical Society · 2018

Pushing Nonlinear Optical Oxides into the Mid-Infrared Spectral Region Beyond 10 μm: Design, Synthesis, and Characterization of La3SnGa5O14

Haichao Lan, Fei Liang, Xingxing Jiang, Cong Zhang, Haohai Yu, Zheshuai Lin, Huaijin Zhang, Jiyang Wang, Yicheng Wu

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Pushing Nonlinear Optical Oxides into the Mid-Infrared Spectral Region Beyond 10 μm: Design, Synthesis, and Characterization of La3SnGa5O14OriginalFirst principle study of nonlinear optical crystals15Optimized oriented seed growth and optical properties of high-quality LiInSe 2 crystals13Research progress of mid-and far-infrared nonlinear optical crystals10Structure Determination of a New Molecular White‐Light Source13Advantageous Units in Antimony Sulfides: Exploration and Design of Infrared Nonlinear Optical Materials95A review on structure-performance relationship toward the optimal design of infrared nonlinear optical materials with balanced performances252Recent advances and future perspectives on infrared nonlinear optical metal halides223Cyano-Based Materials with Giant Optical Anisotropy and Second Harmonic-Generation Effect24Pb 2 GaF 2 (SeO 3 ) 2 Cl: Band Engineering Strategy by Aliovalent Substitution for Enlarging Bandgap while Keeping Strong Second Harmonic Generation Response178Growth, thermal and spectral properties, and laser performance of Tm 3+ :CNGS crystal19“Two in one”: an unprecedented mixed anion, Ba 2 (C 3 N 3 O 3 )(CNO), with the coexistence of isolated sp and sp 2 π-conjugated groups15LiO 4 tetrahedra lock the alignment of π-conjugated layers to maximize optical anisotropy in metal hydroisocyanurates44Rational design of a new chalcogenide with good infrared nonlinear optical performance: SrZnSnS 452Toward terawatt few-cycle pulses via optical parametric chirped-pulse amplification with oxide crystals14Lone‐Pair Enhanced Birefringence in an Alkaline‐Earth Metal Tin(II) Phosphate BaSn 2 (PO 4 ) 2130Ba10In6Zn7S26-nZnS: An Inorganic Composite System with Interface Phase-Matching Tuned for High-Performance Infrared Nonlinear Optical Materials13LiGaP 2 O 7 : A Potential UV Nonlinear-Optical Crystal14Dislocations that Decrease Size Mismatch within the Lattice Leading to Ultrawide Band Gap, Large Second‐Order Susceptibility, and High Nonlinear Optical Performance of AgGaS229Dislocations that Decrease Size Mismatch within the Lattice Leading to Ultrawide Band Gap, Large Second‐Order Susceptibility, and High Nonlinear Optical Performance of AgGaS2186New Members of SHG Active Dugganite Family, A3BC3D2O14 (A = Ba, Pb; B = Te, Sb; C = Al, Ga, Fe, Zn; D = Si, Ge, P, V): Synthesis, Structure, and Materials Properties30Rb7SrY2(B5O10)3: A Rare-Earth Pentaborate with Moderate Second-Harmonic Response and Interesting Phase-Matching Behavior29Interstitial Oxide Ion Conductivity in the Langasite Structure: Carrier Trapping by Formation of (Ga,Ge)2O8 Units in La3Ga5– x Ge1+ x O14+ x /2 (0 < x ≤ 1.5)31LiMII(IO3)3 (MII=Zn and Cd): Two Promising Nonlinear Optical Crystals Derived from a Tunable Structure Model of α‐LiIO398LiMII(IO3)3 (MII=Zn and Cd): Two Promising Nonlinear Optical Crystals Derived from a Tunable Structure Model of α‐LiIO337Rb4Li2TiOGe4O12: A Titanyl Nonlinear Optical Material with the Widest Transparency Range68Rb4Li2TiOGe4O12: A Titanyl Nonlinear Optical Material with the Widest Transparency Range29Rb10Zn4Sn4S17: A Chalcogenide with Large Laser Damage Threshold Improved from the Mn-Based Analogue27Broadband CrOCl Saturable Absorber with a Spectral Region Extension to 10.6 µm33K5(W3O9F4)(IO3): An Efficient Mid-Infrared Nonlinear Optical Compound with High Laser Damage Threshold114A new family of quaternary thiosilicates SrA 2 SiS 4 (A = Li, Na, Cu) as promising infrared nonlinear optical crystals48“Old dog, new tricks”: the lone pair effect inducing divergent optical responses in lead cyanurates containing π-bonds18Li2K4TiOGe4O12: A Stable Mid-Infrared Nonlinear Optical Material69Langasite Family Nonlinear Optical Crystals9Tuning the Langasite, La 3 SbZn 3 Si 2 O 14 , towards white light emission: synthesis, structure, SHG and photoluminescence studies19Infrared Nonlinear Optical Polymorphs α- and β-SrCu 2 SnS 4 Exhibiting Large Second Harmonic Generation Responses with Requisite Phase-Matching Behavior44Lead Mixed Oxyhalides Satisfying All Fundamental Requirements for High‐Performance Mid‐Infrared Nonlinear Optical Materials164Lead Mixed Oxyhalides Satisfying All Fundamental Requirements for High‐Performance Mid‐Infrared Nonlinear Optical Materials55Enhancement of Second-Order Optical Nonlinearity in a Lutetium Selenite by Monodentate Anion Partial Substitution58Flexible inorganic oxide thin-film electronics enabled by advanced strategies19A2SnS5: A Structural Incommensurate Modulation Exhibiting Strong Second‐Harmonic Generation and a High Laser‐Induced Damage Threshold (A=Ba, Sr)30A2SnS5: A Structural Incommensurate Modulation Exhibiting Strong Second‐Harmonic Generation and a High Laser‐Induced Damage Threshold (A=Ba, Sr)86A review on phase transition and structure-performance relationship of second-order nonlinear optical polymorphs107AGa 3 F 6 (SeO 3 ) 2 (A = Rb, Cs): A New Type of Phase-Matchable Hexagonal Tungsten Oxide Material with Strong Second-Harmonic Generation Responses63A 2 Bi 2 (SeO 3 ) 3 F 2 (A = K and Rb): Excellent Mid-Infrared Nonlinear Optical Materials with Both Strong SHG Responses and Large Band Gaps64Pb 18 O 8 Cl 15 I 5 : A Polar Lead Mixed Oxyhalide with Unprecedented Architecture and Excellent Infrared Nonlinear Optical Properties165Pb18O8Cl15I5: A Polar Lead Mixed Oxyhalide with Unprecedented Architecture and Excellent Infrared Nonlinear Optical Properties29Finding Optimal Mid-Infrared Nonlinear Optical Materials in Germanates by First-Principles High-Throughput Screening and Experimental Verification79Recent Advances in Oxide‐based Nonlinear Optical Materials with Wide Infrared Transparency Beyond 6 μm38Intense d ‑ p Hybridization Induced a Vast SHG Response Disparity between Tetrahedral Vanadates and Arsenates13Bi 32 Cd 3 P 10 O 76 : a new congruently melting nonlinear optical crystal with a large SHG response and a wide transparent region24A new broad-band infrared window material CdPbOCl 2 with excellent comprehensive properties10Breaking through the “3.0 eV wall” of energy band gap in mid-infrared nonlinear optical rare earth chalcogenides by charge-transfer engineering144Growth of a large-aperture mid-infrared nonlinear optical La 3 Nb 0.5 Ga 5.5 O 14 crystal for optical parametric chirped-pulse amplification13Heterovalent cations substitution to design asymmetric chalcogenides with promising nonlinear optical performances44Optimized growth and anisotropic properties of Li 2 ZrTeO 6 nonlinear optical crystals8Mid-infrared pulsed nanosecond difference frequency generation of oxide LGN crystal up to 5.7 µm15CsZrF4(IO3): The First Polar Zirconium Iodate with cis-[ZrO2F6] Polyhedra Inducing Optimized Balance of Large Band Gap and Second Harmonic Generation47IR transmission prediction, processing, and characterization of dense La 2 Ce 2 O 710Recent advances in nonlinear optical rare earth structures63A3Te(Zn2Ge)Ge2O14 (A = Sr, Ba, and Pb): New Langasite Mid-infrared Nonlinear Optical Materials by Rational Chemical Substitution32A Congruent‐Melting Mid‐Infrared Nonlinear Optical Vanadate Exhibiting Strong Second‐Harmonic Generation22A Congruent‐Melting Mid‐Infrared Nonlinear Optical Vanadate Exhibiting Strong Second‐Harmonic Generation63Li2MTeO6 (M=Ti, Sn): Mid‐Infrared Nonlinear Optical Crystal with Strong Second Harmonic Generation Response and Wide Transparency Range72Li2MTeO6 (M=Ti, Sn): Mid‐Infrared Nonlinear Optical Crystal with Strong Second Harmonic Generation Response and Wide Transparency Range4CsCdGa3O6: A I-II-III-O (I = alkali metal, II = divalent metal, III = Al, Ga, In) type oxide featuring [Ga4O14]16− helical belts linked [Ga6O6]6+ and [Ga8O8]8+ cages11Ca3(TeO3)2(MO4) (M = Mo, W): Mid-Infrared Nonlinear Optical Tellurates with Ultrawide Transparency Ranges and Superhigh Laser-Induced Damage Thresholds46Polymorphic Pb14O8I12 and Pb7O4I6 oxyhalides featuring unprecedented [O8Pb14] clusters with broad IR transparency20LiNbTeO5: A High-Performance Multifunctional Crystal Material with a Very Large Second-Harmonic Generation Response and Piezoelectric Coefficient52Investigations on the Synthesis, Crystal Structure, Linear- and Nonlinear-Optical Properties of the Zinc Germanate Rb2ZnGe2O627Band gap modulation and nonlinear optical properties of quaternary tellurates Li 2 GeTeO 613K 2 S 4 O 6 : improving birefringence and nonlinear optical properties with the [O 3 S–S–S–SO 3 ] 2− group5Unprecedented mid-infrared nonlinear optical materials achieved by crystal structure engineering, a case study of (KX)P 2 S 6 (X = Sb, Bi, Ba)59HgTeO2F(OH): A Nonlinear Optical Oxyfluoride Constructed of Active [TeO2F(OH)]2– Pyramids and V-Shaped [HgO2]2– Groups36Recent progress on acentric La3Nb0.5Ga5.5O14 crystals: large-size growth and application to ultrafast mid-infrared laser systems [Invited]14Cd4InO(BO3)3: A New Nonlinear Optical Crystal Exhibiting Strong Second Harmonic Generation Effect and Moderate Birefringence2Finding the First Squarates Nonlinear Optical Crystal NaHC4O4·H2O with Strong Second Harmonic Generation and Giant Birefringence56Bi3TeBO9: A Promising Mid-Infrared Nonlinear Optical Crystal with a Large Laser Damage Threshold6Broadband 1T-polytype tantalum disulfide saturable absorber for solid-state bulk lasers10[Ba2F2][Ge2O3S2]: An Unprecedented Heteroanionic Infrared Nonlinear Optical Material Containing Three Typical Anions47Laser damage mechanism and threshold improvement of nonlinear optical La 3 Ga 5.5 Nb 0.5 O 14 crystal for a mid-infrared high-intensity laser12Mixed-Anion-Oriented Design of LnMGa3S6O (Ln = La, Pr, and Nd; M = Ca and Sr) Nonlinear Optical Oxysulfides with Targeted Property Balance56Pb5(GeO4)(Ge2O7) and Pb3.32Ca1.68(GeO4)(Ge2O7): Two Nonlinear Optical Germanates Induced by Diverse PbOx Polyhedra17Tailored Ordered Structures with Functional Units of Distorted [NbO6] and Antiparallel [GeO4] for Enhanced Birefringence in Germanate Crystal15Transparent Lead‐Free Ferroelectric (K, Na)NbO3 Single Crystal with Giant Second Harmonic Generation and Wide Mid‐Infrared Transparency Window21Oxychalcogenides as Promising Ultraviolet Nonlinear Optical Candidates: Experimental and Theoretical Studies of AEGeOS2(AE = Sr and Ba)24Synthesis, structure, characterization, and electronic structure calculation of a new molecule-inclusion strontium gallate Sr6(Ga12O24)·Bi2O32Three polar indium phosphites exhibiting diverse structural networks and SHG-activity9Enhancements of Second Harmonic Generation and Birefringence in Traditional RbTiOPO4‐Type Crystals by Aliovalent Substitution of Ti Site1Oxidation-induced phase transformations of hybrid tin bromide single crystals enable the occurrence of second-harmonic generation14AIB3IIC3IIIQ8VI: A New Family for the Design of Infrared Nonlinear Optical Materials by Coupling Octahedra and Tetrahedra Units152Rb 2 CdSi 4 S 10 : novel [Si 4 S 10 ] T2-supertetrahedra-contained infrared nonlinear optical material with large band gap79Birefringence Dispersion Management of Langasite Nonlinear Crystals for the Improvement of Mid-Infrared Amplification10Insights into molecular cluster materials with adamantane‐like core structures by considering dimer interactions12Recent Advances in Infrared Nonlinear Optical Crystal7KNa 2 La 2 (BO 3 ) 3 : a shortite-type lanthanide borate exhibiting strong nonlinear optical activity induced by isolated [BO 3 ] triangles and distorted [LaO 9 ] polyhedra26LiVTeO 5 : a mid-infrared nonlinear optical vanadium tellurate crystal exhibiting enhanced second harmonic generation activities and notable birefringence21Revisiting two thiophosphate compounds constituting d 0 transition metal HfP 2 S 6 and d 10 transition metal α-Ag 4 P 2 S 6 as multifunctional materials for combining second harmonic generation response and photocurrent response12Intense d‐p Hybridization in Nb3O15 Tripolymer Induced the Largest Second Harmonic Generation Response and Birefringence in Germanates51Intense d‐p Hybridization in Nb3O15 Tripolymer Induced the Largest Second Harmonic Generation Response and Birefringence in Germanates7Unbiased Screening of Novel Infrared Nonlinear Optical Materials with High Thermal Conductivity: Long‐neglected Nitrides and Popular Chalcogenides12Unbiased Screening of Novel Infrared Nonlinear Optical Materials with High Thermal Conductivity: Long‐neglected Nitrides and Popular Chalcogenides48Alignment of Λ-Shaped Basic Building Units to Construct One New KMoO3(IO3) Polar Polymorph11Shooting mid-infrared nonlinear optical materials with targeted balance performances in ternary d0-transition metal oxides through first-principles13Recent progress of newly developed functional building units and corresponding nonlinear optical materials14Cd2Nb2Te4O15: A Novel Pseudo‐Aurivillius‐Type Tellurite with Unprecedented Nonlinear Optical Properties and Excellent Stability40Linear and nonlinear optical properties of the langasite crystal Ca 3 TaAl 3 Si 2 O 143Quadruple‐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 Birefringence2NaCl·CH4N2O·H2O: An Organic–Inorganic Hybrid Ultraviolet Nonlinear Optical Crystal with Optimized Comprehensive Properties8Excellent Nonlinear Optical M[M4Cl][Ga11S20] (M = A/Ba, A = K, Rb) Achieved by Unusual Cationic Substitution Strategy20Preparation and Optical Properties of Nd:Bi2Ti2O7 Laser Crystal with Disordered Structure and Attractive Multiwavelength Emission Characteristics6A comprehensive review of high-transmittance low-conductivity material-assisted radiant cooling air conditioning: Materials, mechanisms, and application perspectives32A defect pyrochlore-like acentric cubic lead titanium-tellurate crystal exhibiting strong second harmonic generation activity and an extended transparent window4Computer-aided screening of bismuth molybdates nonlinear optical crystals γ -Bi 2 MoO 63The Langasite Family for the Development of Oxygen-Vacancy-Mediated Oxide Ion Conductors18Effects of different groups on phase-matching and SHG in “3+4” Pn materials0La3Ga5M0.5Sn0.5O14, (M = Ge, Si): Design and Synthesis of Two Langasite Nonlinear Optical Materials with Large Second Harmonic Generation and Birefringence Induced by Distorted (Sn/M)O6 Octahedra4Bridgman growth and characterizations of nonlinear optical crystal La3Ga5.5Nb0.5O140Directional growth and composition design of the highly disordered Yb3+ doped Ca(Gd1-xLux)AlO4 crystals for ultrafast lasers4Rational Design of Novel Polar Nonlinear Optical Materials in Alkali Metal Rare Earth Iodates5Application of Graphene in Acoustoelectronics0Electron‐Lattice Synergistic Coordination for Boosting the Electro‐Optic Response of the Crystal4AI2Mg3Ga12S22 (AI = K, Rb): T2-type supertetrahedra coupled with [MgS6] octahedra for designing wide-band gap infrared nonlinear optical materials with well-balanced properties16Reinforced 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 116Infrared Absorption Edges in Inorganic Optical Crystals: Understanding and Prediction6La 3 ZrGa 5 O 14 : Band‐Inversion Strategy in Topology‐Protected Octahedron for Large Nonlinear Response and Wide Bandgap18La3ZrGa5O14: Band‐Inversion Strategy in Topology‐Protected Octahedron for Large Nonlinear Response and Wide Bandgap1Two-Step Substitutions of Square Pyramidal VO5 with CdO4Br to Achieve Higher Laser-Induced Damage Threshold from Polar Oxybromides Rb4CdV5O15Br to Rb3CdV4O12Br10Halogen-Driven Structural Engineering in Tellurium Oxyhalides: Enhanced SHG Response and Broad Optical Transparency6Ca 7 (TeO 3 ) 6 (MoO 4 ): A Promising Mid-Infrared Nonlinear Optical Crystal Activated via a Module-Oriented Dimensionality Reduction Strategy34La3Ga5HfO14: Rare-Earth Polyhedron Coupled with Structural Protected Octahedron for Designing Nonlinear Optical Material with Wide Bandgap and Well-Balanced Properties5Halogen-Tuned BiOX (X = Cl, Br, I) Layered Crystals with Superior Broadband Nonlinear Saturable Absorption for Pulsed Laser Modulation2CsICl 2 : A Record-Birefringent Inorganic Crystal with Ultrawide Infrared Transparency Enabled by Linear Interhalogen ICl 2 – Units36Optimized growth and anisotropic physical properties of a promising mid-infrared nonlinear optical crystal Li2TiTeO63A Band‐Orientation Co‐Anchoring Strategy for the Design of a High‐Performance Mid‐Infrared Nonlinear Optical Crystal2A Band‐Orientation Co‐Anchoring Strategy for the Design of a High‐Performance Mid‐Infrared Nonlinear Optical Crystal12A series of langasite-type compounds: size effect regulation for cation occupation and enhanced SHG response1Synthesis, structure, and luminescence properties of a novel Langasite-type La2BaGa4Si2O14:Eu3+ red phosphor0中红外氧化物非线性光学晶体研究进展（特邀）0Local Rigid-Unit Design Modulates Interstitial Oxygen Coordination Geometry for Developing Langasite-Type Oxide-Ion Solid Electrolytes2Rational design of a quasi-0D tungsten tellurite nonlinear optical crystal with exceptionally balanced properties1Quasi-degenerate cation occupation enables nearly defect-free functional crystals0First‐Principles Investigation of the Structural, Electronic, Optical, Elastic, and Thermal Properties of Defect Diamond‐Like Hg 3 P 2 S 80Synthesis, structure, and luminescence properties of a novel langasite-type La2BaGa4Si2O14:Eu3+ red phosphor0

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  4. Structure Determination of a New Molecular White‐Light Source

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  5. Advantageous Units in Antimony Sulfides: Exploration and Design of Infrared Nonlinear Optical Materials

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  6. A review on structure-performance relationship toward the optimal design of infrared nonlinear optical materials with balanced performances

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  7. Recent advances and future perspectives on infrared nonlinear optical metal halides

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  12. LiO 4 tetrahedra lock the alignment of π-conjugated layers to maximize optical anisotropy in metal hydroisocyanurates

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  13. Rational design of a new chalcogenide with good infrared nonlinear optical performance: SrZnSnS 4

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  30. A new family of quaternary thiosilicates SrA 2 SiS 4 (A = Li, Na, Cu) as promising infrared nonlinear optical crystals

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  31. “Old dog, new tricks”: the lone pair effect inducing divergent optical responses in lead cyanurates containing π-bonds

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  32. Li2K4TiOGe4O12: A Stable Mid-Infrared Nonlinear Optical Material

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  33. Langasite Family Nonlinear Optical Crystals

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  34. Tuning the Langasite, La 3 SbZn 3 Si 2 O 14 , towards white light emission: synthesis, structure, SHG and photoluminescence studies

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  35. Infrared Nonlinear Optical Polymorphs α- and β-SrCu 2 SnS 4 Exhibiting Large Second Harmonic Generation Responses with Requisite Phase-Matching Behavior

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  36. Lead Mixed Oxyhalides Satisfying All Fundamental Requirements for High‐Performance Mid‐Infrared Nonlinear Optical Materials

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  38. Enhancement of Second-Order Optical Nonlinearity in a Lutetium Selenite by Monodentate Anion Partial Substitution

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  39. Flexible inorganic oxide thin-film electronics enabled by advanced strategies

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  40. A2SnS5: A Structural Incommensurate Modulation Exhibiting Strong Second‐Harmonic Generation and a High Laser‐Induced Damage Threshold (A=Ba, Sr)

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  41. A2SnS5: A Structural Incommensurate Modulation Exhibiting Strong Second‐Harmonic Generation and a High Laser‐Induced Damage Threshold (A=Ba, Sr)

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  42. A review on phase transition and structure-performance relationship of second-order nonlinear optical polymorphs

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  43. AGa 3 F 6 (SeO 3 ) 2 (A = Rb, Cs): A New Type of Phase-Matchable Hexagonal Tungsten Oxide Material with Strong Second-Harmonic Generation Responses

    Chemistry of Materials · 2020-06-23

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  44. A 2 Bi 2 (SeO 3 ) 3 F 2 (A = K and Rb): Excellent Mid-Infrared Nonlinear Optical Materials with Both Strong SHG Responses and Large Band Gaps

    Chemistry of Materials · 2020-08-21

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  45. Pb 18 O 8 Cl 15 I 5 : A Polar Lead Mixed Oxyhalide with Unprecedented Architecture and Excellent Infrared Nonlinear Optical Properties

    Angewandte Chemie International Edition · 2020-09-02

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  46. Pb18O8Cl15I5: A Polar Lead Mixed Oxyhalide with Unprecedented Architecture and Excellent Infrared Nonlinear Optical Properties

    Angewandte Chemie · 2020-09-02

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  47. Finding Optimal Mid-Infrared Nonlinear Optical Materials in Germanates by First-Principles High-Throughput Screening and Experimental Verification

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  48. Recent Advances in Oxide‐based Nonlinear Optical Materials with Wide Infrared Transparency Beyond 6 μm

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  49. Intense d ‑ p Hybridization Induced a Vast SHG Response Disparity between Tetrahedral Vanadates and Arsenates

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  50. Bi 32 Cd 3 P 10 O 76 : a new congruently melting nonlinear optical crystal with a large SHG response and a wide transparent region

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