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RESEARCH ARTICLE · Advanced Materials · 2023

Target‐Driven Design of Deep‐UV Nonlinear Optical Materials via Interpretable Machine Learning

Mengfan Wu, Evgenii Tikhonov, Abudukadi Tudi, Ivan A. Kruglov, Xueling Hou, Congwei Xie, Shilie Pan, Zhihua Yang

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Target‐Driven Design of Deep‐UV Nonlinear Optical Materials via Interpretable Machine LearningOriginalMg 2 Pb 2 Si 2 O 7 F 2 : a new lead-containing alkali earth metal silicate fluoride with a short cutoff edge2Mg assists in modulating the dimensionalities of the anionic frameworks of borates1Recent progress in borate-based short-wavelength nonlinear optical crystals with boron–oxygen skeleton modification28Target-Oriented Synthesis of Borate Derivatives Featuring Isolated [B3O3] Six-Membered Rings as Structural Features20Multidimensional modelling and designing of efficient small molecule acceptors for organic solar cells4Closed‐Loop Error‐Correction Learning Accelerates Experimental Discovery of Thermoelectric Materials14Li2RbSO4Cl with a Short Ultraviolet Absorption Edge and an Acentric Structure through Assembling Heteroleptic [LiO3Cl] Tetrahedra2Three Borates Belonging to the A(I)7Ae(II)Re(III)2B15O30 Family as Promising Nonlinear Optical Crystals12ACd 4 Ga 5 Te 12 (A = K, Rb, Cs): Tellurides with a Strong Nonlinear Optical Response and Purple Emission24A Machine Learning Study on High Thermal Conductivity Assisted to Discover Chalcogenides with Balanced Infrared Nonlinear Optical Performance58Vanadate Crystals with an Enhanced Birefringence and a Broadened Transparency Spectrum through Controlled [VO3]∞ Chain Arrangements and Alkali Metal Cation Introduction4Interpretable Machine Learning‐Assisted High‐Throughput Screening for Understanding NRR Electrocatalyst Performance Modulation between Active Center and C‐N Coordination59Cd8(BO3)4SiO4: Metal Cation Inducing the Formation of Isolated [BO3] and [SiO4] Units in Borate Silicate15A UV non-hydrogen pure selenite nonlinear optical material for achieving balanced properties through framework-optimized structural transformation41K, Rb-hydroxyborates series with deep-ultraviolet KRbB 5 O 8 (OH) possessing moderate second harmonic generation response0Machine learning-assisted high-throughput screening of transparent organic light-emitting diode anode materials17Multi-fidelity machine learning for predicting bandgaps of nonlinear optical crystals14Recent advances in rational structure design for nonlinear optical crystals: leveraging advantageous templates153Research progress in optical materials with cationic organic planar π-conjugated groups containing CN bonds34Shooting short-wavelength nonlinear optical materials with targeted balance performances in hydroxyborates through first-principles high-throughput screening4Structural strategy for advancing nonlinear optical effects in 1D-[MX 2 ] ∞ chains: internal distortion and atomic types2Screening Large Birefringent Materials via Halogen Regulation in Ternary d0-Transition Metal Oxyhalides8Synthesis, structures and properties of two new nitrate optical materials: Rb3ZnNO3Cl4 and Rb5Na(NO3)4Cl24The Birefringence Modulation in Short‐Wave Ultraviolet Sulfates with Functional π‐Conjugated Cations and Polymerized Heteroleptic Tetrahedral Anions18Dual-Anion Strategy Induces Dual Enhancement Toward Ultrashort Phase-Matching Wavelength in Deep-UV Transparent d0 Transition Metal Oxyfluorides21A perspective on deep-ultraviolet nonlinear optical materials13Vacancy‐Induced Extraordinary Second Harmonic Generation Response for Diamond‐Like Cu3PS49Layered (C5H6ON)2[Sb2O(C2O4)3] with a large birefringence derived from the uniform arrangement of π-conjugated units11Two Hydroxyfluorooxoborates Achieving Deep‐Ultraviolet Cutoff Edges and Moderate Birefringence by Assembling Multi‐Anionic Groups6A Universal Design Strategy Achieving Large Birefringence and Short Phase‐Matching Capability of Optical Materials via Dissimilating Non‐π‐Conjugated Units6Enhanced Birefringence in Phosphates via “Two Steps in One”: d0 Transition Metal Regulation and Fluorination Synergistic Strategy7Accelerating the discovery of direct bandgap doped-spinel photovoltaic materials: A target-driven approach using interpretable machine learning7Room-Temperature Phase Transition Material with Switchable Second-Order Nonlinear Optical Properties9Machine learning regression model for predicting the band gap of multi-elements nonlinear optical crystals17The Application of Supervised Learning Algorithms in Predicting the Formation Energy of NLO Crystals3Review on birefringence in borates based on birefringence-active functional groups and arrangements57Accurate prediction of second harmonic generation coefficients using graph neural networks11Fluorine-driven materials design of novel deep-ultraviolet nonlinear optical crystal materials: Research progress and challenges6A Machine-Learning-Assisted Crystalline Structure Prediction Framework To Accelerate Materials Discovery19Inverse Design of Low-Resistivity Ternary Gold Alloys via Interpretable Machine Learning and Proactive Search Progress2Sulfate Derivatives with Heteroleptic Tetrahedra: New Deep‐Ultraviolet Birefringent Materials in which Weak Interactions Modulate Functional Module Ordering61Sulfate Derivatives with Heteroleptic Tetrahedra: New Deep‐Ultraviolet Birefringent Materials in which Weak Interactions Modulate Functional Module Ordering4Inverse design of a novel multiport power divider based on hybrid neural network0Data‐Driven Materials Research and Development for Functional Coatings120Exploiting 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 ] Groups4From B 3 O 3 (OH) 3 to B 3 O 3 F 3 : Uncovering Series of New Functional Units Based on [BO 2 F] Beneficial for Deep‐Ultraviolet Birefringence1Learning From Nature: The Rational Non‐Centrosymmetric Structural Design in the Honeycomb‐Like Gaudefroyite Family23The design of a non-centrosymmetric structure in sulfates by cation-induced symmetry breaking4Rb 1.87 Cs 1.13 B 8 O 13 (NO 3 ): a new acentric borate-nitrate with two types of three-dimensional interpenetrating lattices1Computer‐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 enhancement1Data driven design of dyes with high dielectric constant for efficient optoelectronics3“AI+光学”交叉学科体系的内涵与架构研究（特邀）0(CN 4 H 7 ) 2 SO 4 ·H 2 O: high-performance metal-free ultraviolet birefringent crystal with KBBF-like configuration5Anion ratio-directed design of CaB 4 O 5 F 4 and CaB 6 O 8 F 4 : [BO 3 ]/[BO 2 F 2 ] hybridization tailoring deep-ultraviolet nonlinear optical performance2BaSbBS 4 : a record-high-performance birefringent crystal identified by a target-driven closed-loop strategy28Exploration of nonlinear optical materials by introducing information science4Li 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 waveplates4M 3 MoO 4 (HCO 3 ) (M = Rb and Cs): cation-tuned synthesis of two noncentrosymmetric molybdate-carbonates with isolated [MoO 4 ] and [HCO 3 ] groups0Non-centrosymmetric structures designed rationally via a “dimensionality addition” strategy toward the promising nonlinear optical family [A–X][In–Se] (A = K/Ba and Rb/Ba; X = Cl and Br)13新型非线性光学晶体和双折射晶体的研究进展（特邀）4混合阴离子无水无机硼酸盐深紫外非线性光学晶体的研究进展（特邀）4Artificial intelligence-driven phase stability evaluation and new dopants identification of hafnium oxide-based ferroelectric materials26A Cu(I)-Based MOF with Nonlinear Optical Properties and a Favorable Optical Limit Threshold6Accelerating Discovery of Infrared Nonlinear Optical Materials with High Lattice Thermal Conductivity: Combining Machine Learning and First‐Principles Calculations10AI-empowered digital design of zeolites: Progress, challenges, and perspectives15Machine Learning-Assisted Accelerated Research of Energy Storage Properties of BaTiO3–BiMeO3 Ceramics9Strong Second‐Harmonic Generation Responses in Salt‐Inclusion Oxychalcogenides Enabled by the Highly Distorted Polyhedra with Mixed‐Anions4The birefringence in orthorhombic and triclinic lead-iodates and the functional basic units' contribution: A first-principles investigation3K2PbB5P3O17: A Mixed-Coordinated Borophosphate with Enhanced Birefringence Driven by the [B2O5] Unit5Prediction of New Functional Fluorooxoborates with Expected Anionic Framework: A Case of CaB3O5F4The effect of hydrostatic pressure on the electronic structure and elastic properties of ZGP and CGP crystals0La 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 Bandgap1Data‐Driven Design of Spinodal Decomposition in (Ti, Zr, Hf)C Composite Carbides for Optimizing the Hardness‐Toughness Trade‐Off6AI4NLO: An Integrated Data Platform for Machine Learning-Driven Exploration of Inorganic Nonlinear Optical Materials8Hierarchy-boosted funnel learning for identifying semiconductors with ultralow lattice thermal conductivity8Synergistic Machine Learning Guided Discovery of ABa 3 (BSe 3 ) 2 X (A = Rb, Cs; X = Cl, Br, I): A Promising Family as Property‐Balanced IR Functional Materials10Ba2BeB2O6: A True Zero-Order Waveplate Material with Minimal Birefringence Achieved via Structural Regulation2Improving the Performance of Birefringent Crystals by Molecular Assembly Strategy in the Solar‐Blind UV Region14Biomimetic Intelligent Thermal Management Materials: From Nature‐Inspired Design to Machine‐Learning‐Driven Discovery50Non-equivalent terminating roles of hydroxyl and fluorine in hydroxy/fluorooxo-borate optical functional materials2Machine Learning Prediction on Birefringence of Nonlinear Optical Crystals and Polymorphs with Different Birefringence Activities2Unravelling the impact of octahedral distortion and non-covalent interactions on the hyperpolarizabilities of Co(II) and Ni(II) coordination complexes with uridine nucleotide11Reversal Enhancement of Birefringence by Stereochemically Active Lone Pairs in Sn(II)-Based Mixed Halides0La(SO3NH2)2NO3·H2O: synergistic anion engineering of the first rare-earth nitrate sulfamate defying transparency-birefringence-nonlinearity trade-offs in ultraviolet nonlinear optics8[HgX 2 ] Linear Group Enabled Ultraviolet Birefringent Crystal RbHg 5 Br 11 with Strong Optical Anisotropy and Wide Bandgap12Quinolone-functionalized glycine dipeptides: TPA enhancement and charge transfer mechanism2Two-dimensional graphene-like BeO sheet: a promising deep-ultraviolet nonlinear optical material with strong and highly tunable second harmonic generation5Symmetry‐Aware Equivariant Network for Discovering SHG‐Active Materials5Tuning birefringence in alkaline-earth metal oxyhalides through diverse mixed-cation coordination architectures1High‐Throughput Discovery of Large Birefringence Materials in Mixed‐N Hf‐O Systems0Heterocationic strategy to design a nonlinear optical crystal with a polar anti-perovskite structure7[C(NH 2 ) 3 ] 2 PO 3 (OH): A Deep-Ultraviolet Birefringent Crystal Enabled by Synergy of π-Conjugated Cations and Heteroleptic Tetrahedra2Novel [BO 2 ] superhalogen module-enabled deep-ultraviolet nonlinear optical material: rational design for tailored birefringence and phase matching0Navigating the Landscape of Next-Generation Nonlinear Optical Materials Discovery: Opportunities and Challenges Driven by Artificial Intelligence4A series of langasite-type compounds: size effect regulation for cation occupation and enhanced SHG response1Design rules for nonlinear optical materials: dimensionality, interfaces, topological band geometry and data-driven discovery2Interpretable machine learning-assisted discovery of BaTiO 3 -based ceramics with enhanced dielectric constant1Synergistic dual-modification strategy of π-conjugated cations and tetrahedra: rational design of ultraviolet high-birefringence monofluorophosphates0Targeted hydroxyl fluorination for first-principles design of deep-ultraviolet nonlinear optical crystals: multi-property optimization & chromatic dispersion modulation in Li 2 CsB 7 O 10 F 41Two scandium borate UV NLO crystals designed through chemical element substitution1Identifying the Catalytic Descriptor of Single-Atom Catalysts in Nitrate Reduction Reaction: An Interpretable Machine-Learning Method18Functional Unit Design of Deep‐UV NLO Crystals With Short Phase‐Matching and Large SHG Response22Atmospheric Corrosion Prediction of Low-Alloy Carbon Steel Based on Dual-Correction Dynamic Ensemble Framework0Machine learning-assisted optical thermometry with carbon dots: photophysical foundations and intelligent temperature sensing0Hydrogen‐Bond‐Directed Assembly of Urea Derivatives: Exceptional Birefringence Achieved by π ‐Conjugated Unit Alignment3Interpretable Machine Learning for Bandgap Prediction and Descriptor‐Guided Design Rules of Phosphates1High‐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 Verification2Accelerated Discovery of Fluorophosphates as Deep‐Ultraviolet Nonlinear Optical Materials in the Y–P–O–F System: Unveiling New Composition‐Structure‐Property Rules1An Integrated Machine Learning Workflow Based on Deep Generative Models for Discovery of Inorganic Nonlinear Optical Crystals0Giant Birefringence and Ultrahigh Thermal Conductivity in Layered MgMoN 20Gravity‐Field Self‐Regulatory Engineering Enables PbIn 6 Te 10 Nonlinear Optical Crystals Boosting Laser‐Induced Damage Threshold1Interpretable machine learning for tensile strength prediction and processing optimization of thermoplastic vulcanizates0Donor–Acceptor Covalent Organic Frameworks with Modulated Excitonic Effects for Enhanced Nonlinear Optical Responses0Artificial intelligence for carbon materials in electrochemical energy storage: Methods, applications, and perspectives0Exceptional Solar‐Blind Birefringence Engineered by Complementary Hydrogen‐Bond Ordering of π‐Conjugated Units0Machine learning-guided multi-parameter performance prediction and screening for anion exchange membrane fuel cell0Accelerating the Discovery of Deep-Ultraviolet Nonlinear Optical Materials by Combining Machine Learning Interatomic Potentials with First-Principles Calculations: A Case of LiB2O3F0Rational Design of a Strong Nonlinear Optical Crystal With Ultrawide Bandgap via Fine‐Tuning of Channel Structures0Machine learning predictions of optical properties in metal-organic complexes: linear and nonlinear constants0Short-UV Metal Halide Nitrates: Moderate SHG in K3Sb(NO3)3F3 and Enhanced Optical Anisotropy in K3Zn(NO3)X4 (X = Cl, Br)0

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  4. Target-Oriented Synthesis of Borate Derivatives Featuring Isolated [B3O3] Six-Membered Rings as Structural Features

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  46. Exploiting Deep‐Ultraviolet Nonlinear Optical Material Rb 2 ScB 3 O 6 F 2 Originated from Congruously Oriented [B 3 O 6 ] Groups

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  48. Learning From Nature: The Rational Non‐Centrosymmetric Structural Design in the Honeycomb‐Like Gaudefroyite Family

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  49. The design of a non-centrosymmetric structure in sulfates by cation-induced symmetry breaking

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  50. Rb 1.87 Cs 1.13 B 8 O 13 (NO 3 ): a new acentric borate-nitrate with two types of three-dimensional interpenetrating lattices

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