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RESEARCH PAPER · ACS Applied Materials & Interfaces · 2020

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

Jin Yu, Bingbing Zhang, Xiaodong Zhang, Ying Wang, Kui Wu, Ming‐Hsien Lee

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Finding Optimal Mid-Infrared Nonlinear Optical Materials in Germanates by First-Principles High-Throughput Screening and Experimental VerificationOriginalFrom silicates to oxonitridosilicates: improving optical anisotropy for phase-matching as ultraviolet nonlinear optical materials47Two Lead Halides with Strong SHG Response Obtained by the Isovalent Substitutions of Alkali Metal Cation and Halogen Anion22Alloy Engineering of a Polar (Si,Ge)2N2O System for Controllable Second Harmonic Performance7Li 4 MgGe 2 S 7 : The First Alkali and Alkaline‐Earth Diamond‐Like Infrared Nonlinear Optical Material with Exceptional Large Band Gap213Li4MgGe2S7: The First Alkali and Alkaline‐Earth Diamond‐Like Infrared Nonlinear Optical Material with Exceptional Large Band Gap15The application and development of the first principles calculation in nonlinear optical materials1CsCdGa3O6: 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+ cages11Machine Learning with Multilevel Descriptors for Screening of Inorganic Nonlinear Optical Crystals35From CeF2(SO4)·H2O to Ce(IO3)2(SO4): Defluorinated Homovalent Substitution for Strong Second-Harmonic-Generation Effect and Sufficient Birefringence53Hg-based chalcogenides: An intriguing class of infrared nonlinear optical materials128Investigations on the Synthesis, Crystal Structure, Linear- and Nonlinear-Optical Properties of the Zinc Germanate Rb2ZnGe2O627Linear unit BN 2 : a novel birefringence-enhanced fundamental module with sp orbital hybridization9Stability and fundamental properties of Cu x O 1− x as optoelectronic functional materials4Synthesis, Structure Determination, and Characterizations of a Polar Salt-Inclusion Scandium Germanate, Rb10Li3Sc4Ge12O36F7Review of Heteroleptic Tetrahedra as Birefringent or Nonlinear Optical Motifs17Phosphogermanate Crystal: A New Ultraviolet–Infrared Nonlinear Optical Crystal with Excellent Optical Performances16Machine learning in computational chemistry7The Combination of Structure Prediction and Experiment for the Exploration of Alkali‐Earth Metal‐Contained Chalcopyrite‐Like IR Nonlinear Optical Material104Assessment of alkali and alkaline earth metals doped cubanes as high-performance nonlinear optical materials by first-principles study29Screening Nitrides with High Debye Temperatures as Nonlinear Optical Materials19Exploring the Stability of Single-Atom Catalysts Using the Density Functional Theory-Based Global Optimization Method: H2 Formation on VOx/γ-Al2O3(100)12Shedding Light on the Structure and Characterization of K2ZnGe2O6: A Phase-Matchable Nonlinear Optical Crystal19Pb5(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 Crystal15Three polar indium phosphites exhibiting diverse structural networks and SHG-activity9Optimal high-throughput virtual screening pipeline for efficient selection of redox-active organic materials7A new infrared nonlinear optical material BaZnGeS 4 with a wide band gap and large nonlinear optical response34Achieving broadband ultraviolet to mid-infrared transparency in germanate-based nonlinear optical crystals Cs 3 REGe 3 O 9 (RE = Y, Gd)16Deciphering the photocatalytic hydrogen generation process of Fresnoite Ba 2 TiGe 2 O 8 by electronic structure and bond analyses9Searching for silicate nonlinear optical materials by combining calculation and experiment17Intense 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 Germanates7Rational 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 System15Unbiased 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 Chalcogenides48Shooting mid-infrared nonlinear optical materials with targeted balance performances in ternary d0-transition metal oxides through first-principles13Semiconducting nonperovskite ferroelectric oxynitride designed ab initio1Machine Learning Classification Model for Screening of Infrared Nonlinear Optical Crystals6(NH4)3(H3O)Zn4(PO4)4: A nonlinear optical zinc orthophosphate crystal9Zn 2 HgP 2 S 8 : A Wide Bandgap Hg‐Based Infrared Nonlinear Optical Material with Large Second‐Harmonic Generation Response75AlphaMat: a material informatics hub connecting data, features, models and applications52Optimal decision-making in high-throughput virtual screening pipelines11A Machine Learning Study on High Thermal Conductivity Assisted to Discover Chalcogenides with Balanced Infrared Nonlinear Optical Performance58Ag 2 [TeO 2 (OH) 4 ]: a nonlinear optical tellurate with balanced comprehensive performance2Computer-aided screening of bismuth molybdates nonlinear optical crystals γ -Bi 2 MoO 63Multi-fidelity machine learning for predicting bandgaps of nonlinear optical crystals14Predictive nonlinear optical crystal formation energy regression model based on convolutional neural networks5Rare-earth-based chalcogenides and their derivatives: an encouraging IR nonlinear optical material candidate70Rb 8 Nb 10 Ge 6 O 41 : a new niobium-germanate crystal featuring unique one-dimensional [Nb 7 O 30 ] ∞ chains and wide mid-IR transparency2Synthesis and Properties Study of a Germanate Mid-Infrared Nonlinear Optical Crystal0Unearthing Superior Inorganic UV Second‐Order Nonlinear Optical Materials: A Mineral‐Inspired Method Integrating First‐Principles High‐Throughput Screening and Crystal Engineering124Unearthing Superior Inorganic UV Second‐Order Nonlinear Optical Materials: A Mineral‐Inspired Method Integrating First‐Principles High‐Throughput Screening and Crystal Engineering4Absorption and emission properties of Eu3+ doped Cs2Bi2O(Ge2O7) acentric biaxial single crystal3Li13YGe4O16: A Mid-infrared Rare-Earth Germanate Nonlinear Optical Crystal Featuring a Broad Transmission Range and an Enlarged Band Gap10HgC4H4O6: A mercury tartrate exhibits phase matchable second harmonic generation effect1Second-harmonic generation tensors from high-throughput density-functional perturbation theory15La3Ga5M0.5Sn0.5O14, (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 Octahedra4DFT Study on the Second-Order NLO Responses of 2-Phenyl Benzoquinoline Ir(III) Complexes by Substituents and Redox Effects1Computer‐Aided Development of New Nonlinear Optical Materials38Computer‐Aided Development of New Nonlinear Optical Materials14Emergent Mid‐Infrared Nonlinear Optical Candidates With Targeted Balance Performances17Accelerating the discovery of high-performance nonlinear optical materials using active learning and high-throughput screening11Exploration of nonlinear optical materials by introducing information science4Prediction and Evaluation of Li 2 ZnS 2 Crystals as Mid‐Infrared Nonlinear Optical Material with High Thermal Conductivity7Two-Step Substitutions of Square Pyramidal VO5 with CdO4Br to Achieve Higher Laser-Induced Damage Threshold from Polar Oxybromides Rb4CdV5O15Br to Rb3CdV4O12Br10AI4NLO: An Integrated Data Platform for Machine Learning-Driven Exploration of Inorganic Nonlinear Optical Materials8First-Principles High-Throughput Screening Combined with Experimental Synthesis to Find Vanadate Nonlinear Optical Material BiCa2VO64Machine Learning Prediction on Birefringence of Nonlinear Optical Crystals and Polymorphs with Different Birefringence Activities2Tuning birefringence in alkaline-earth metal oxyhalides through diverse mixed-cation coordination architectures1A promising mid-infrared nonlinear optical crystal with well-balanced properties0A series of langasite-type compounds: size effect regulation for cation occupation and enhanced SHG response1LnMg 6 Ga 6 S 16 (Ln = Nd, Sm), two bifunctional optical materials exhibiting both nonlinear optical and photoluminescent properties0Normalized Descriptor for Unbiased Screening of Second-Order Nonlinear Optical Materials3K 3 YGe 3 O 9 : A Rare-Earth Germanate Nonlinear Optical Crystal with a Short Ultraviolet Cutoff Edge and Moderate Second-Harmonic Generation Response1A Polar Cerium Iodate Ce 2 (IO 3 ) 6 (H 2 O) with a Strong Second-Harmonic Generation Response in Trivalent Ce-Based Materials1Crystal Growth, Structure and Optical Properties of (NH 4 ) 2 Mg(SO 4 ) 2 ·6H 2 O: A Crystal With a Wide Deep Ultraviolet Window0High‐Performance Infrared Nonlinear Optical Crystals Discovery Guided by High‐Throughput Computation, Machine Learning, and Experimental Verification6High‐Performance Infrared Nonlinear Optical Crystals Discovery Guided by High‐Throughput Computation, Machine Learning, and Experimental Verification2Machine-Learning Discovery of Metal–Organic Framework Crystals for Second-Harmonic Generation0

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  2. Two Lead Halides with Strong SHG Response Obtained by the Isovalent Substitutions of Alkali Metal Cation and Halogen Anion

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  3. Alloy Engineering of a Polar (Si,Ge)2N2O System for Controllable Second Harmonic Performance

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  4. Li 4 MgGe 2 S 7 : The First Alkali and Alkaline‐Earth Diamond‐Like Infrared Nonlinear Optical Material with Exceptional Large Band Gap

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  5. Li4MgGe2S7: The First Alkali and Alkaline‐Earth Diamond‐Like Infrared Nonlinear Optical Material with Exceptional Large Band Gap

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  6. The application and development of the first principles calculation in nonlinear optical materials

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  7. CsCdGa3O6: 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+ cages

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  9. From CeF2(SO4)·H2O to Ce(IO3)2(SO4): Defluorinated Homovalent Substitution for Strong Second-Harmonic-Generation Effect and Sufficient Birefringence

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  10. Hg-based chalcogenides: An intriguing class of infrared nonlinear optical materials

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

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  16. Phosphogermanate Crystal: A New Ultraviolet–Infrared Nonlinear Optical Crystal with Excellent Optical Performances

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  19. Assessment of alkali and alkaline earth metals doped cubanes as high-performance nonlinear optical materials by first-principles study

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  44. Ag 2 [TeO 2 (OH) 4 ]: a nonlinear optical tellurate with balanced comprehensive performance

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  45. Computer-aided screening of bismuth molybdates nonlinear optical crystals γ -Bi 2 MoO 6

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  48. Rare-earth-based chalcogenides and their derivatives: an encouraging IR nonlinear optical material candidate

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  49. Rb 8 Nb 10 Ge 6 O 41 : a new niobium-germanate crystal featuring unique one-dimensional [Nb 7 O 30 ] ∞ chains and wide mid-IR transparency

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