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RESEARCH PAPER · Materials Horizons · 2021

Breaking through the “3.0 eV wall” of energy band gap in mid-infrared nonlinear optical rare earth chalcogenides by charge-transfer engineering

Dajiang Mei, Wangzhu Cao, Naizheng Wang, Xingxing Jiang, Jun Zhao, Weikang Wang, Junhui Dang, Shiyan Zhang, Yuandong Wu, Pinhua Rao, Zheshuai Lin

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Breaking through the “3.0 eV wall” of energy band gap in mid-infrared nonlinear optical rare earth chalcogenides by charge-transfer engineeringOriginalApplying band gap engineering to tune the linear optical and nonlinear optical properties of noncentrosymmetric chalcogenides La 4 Ge 3 Se x S 12− x ( x = 0, 2, 4, 6, 8, 10)21Ba 2 Ge 2 Te 5 : a ternary NLO-active telluride with unusual one-dimensional helical chains and giant second harmonic-generation tensors31SnPQ3 (Q = S, Se, S/Se): A Series of Lone-Pair Cationic Chalcogenophosphates Exhibiting Balanced NLO Activity Originating from SnQ8 Units49The Rise of Infrared Nonlinear Optical Pnictides: Advances and Outlooks36Synthesis, Crystal Structure, and Nonlinear Optical Property of an Anhydrous Sulfate KTb(SO4)216Syntheses, Structures and Properties of Alkali and Alkaline Earth Metal Diamond-Like Compounds Li2MgMSe4 (M = Ge, Sn)12Dimensionality reduction made high-performance mid-infrared nonlinear halide crystal74Noncentrosymmetric Ba6In2Q10 (Q = S, Se): Structural Chemistry and Nonlinear-Optical Activity11Noncentrosymmetric chalcohalide K2Ba3Ge3S9Cl2: A new nonlinear optical material with remarkable laser-induced damage threshold17Halogen-Ion-Induced Structural Phase Transition Giving a Polymorph of HgBr2 with Balanced Nonlinear Optical Properties8Complex coordinated functional groups: A great genes for nonlinear optical materials64Ba2B13O19(OH)5·5H2O: A promising nonlinear optical material with a unique 2[B13O19(OH)5]∞ two-dimensional layer9Noncentrosymmetric (KBa0.5)In2Se4 and (K0.58Ba0.71)(Ga0.89In1.11)Se4 derived from centrosymmetric BaIn2Se4 via partial cation substitution: structural chemistry and nonlinear optical activity9Pnictides: An emerging class of infrared nonlinear optical material candidates47Partial congener substitution induced centrosymmetric to noncentrosymmetric structural transformation and nonlinear optical properties of PbSnSiS413AAg 2 PS 4 (A = K, Na/K): the first-type of noncentrosymmetric alkali metal Ag-based thiophosphates exhibiting excellent second-order nonlinear optical performances21Alkali metal partial substitution-induced improved second-harmonic generation and enhanced laser-induced damage threshold for Ag-based sulfides21Ba 4 Ag 5 (IO 3 ) 6 (I 3 O 8 ) 3 (I 4 O 11 ) 2 : a nonlinear optical crystal containing two types of polyiodate anions16Centrosymmetric Rb[Te 2 O 4 (OH) 5 ] and noncentrosymmetric K 2 [Te 3 O 8 (OH) 4 ]: metal tellurates with corner and edge-sharing (Te 4 O 18 ) 12− anion groups8Na 4 Ga 8 S 14 : a Ga-enriched wide band gap ternary alkali-metal sulfide with unique [Ga 12 S 42 ] 12-membered rings2New Quaternary Sulfide LiGaSiS 4: Synthesis, Structure and Optical Properties0Symmetry breaking of A 3 M 2 X 9 -type perovskite derivatives induced by polar quaternary ammonium cations: achieving efficient nonlinear optical properties28Two new tellurite halides with cationic layers: syntheses, structures, and characterizations of CdPb 2 Te 3 O 8 Cl 2 and Cd 13 Pb 8 Te 14 O 42 Cl 1418Two-step nonlinear optical switch in a hydrogen-bonded perovskite-type crystal15Unprecedented mid-infrared nonlinear optical materials achieved by crystal structure engineering, a case study of (KX)P 2 S 6 (X = Sb, Bi, Ba)59Quaternary Noncentrosymmetric Rare-Earth Sulfides Ba4RE2Cd3S10 (RE = Sm, Gd, or Tb): A Joint Experimental and Theoretical Investigation17HgTeO2F(OH): A Nonlinear Optical Oxyfluoride Constructed of Active [TeO2F(OH)]2– Pyramids and V-Shaped [HgO2]2– Groups36SrZnSnSe4: A quaternary selenide with large second harmonic generation and birefringence39Ba6(CuxZy)Sn4S16 (Z = Mg, Mn, Zn, Cd, In, Bi, Sn): High Chemical Flexibility Resulting in Good Nonlinear-Optical Properties12Phosphogermanate Crystal: A New Ultraviolet–Infrared Nonlinear Optical Crystal with Excellent Optical Performances16Strong 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)2212Synthesis, Crystal and Electronic Structures, and Nonlinear Optical Properties of Y4Si3S1212Crystal Growth, Characterization, and Thermal Annealing of Nonlinear Optical Crystals AgGaGenSe2(n+1) (n = 1.5, 1.75, 2, 3, 4, 5, and 9) for Mid-infrared Applications12New quaternary sulfide LiGaSiS4: Synthesis, structure and optical properties0Rb2FeGe3S8 and Cs2FeGe3S8: New layered chalcogenides in A2MIIMIV3Q8 family with antiferromagnetic property6AgGaGeSe4: An Infrared Nonlinear Quaternary Selenide with Good Performance6(Na0.74Ag1.26)BaSnS4: A New AgGaS2‐Type Nonlinear Optical Sulfide with a Wide Band Gap and High Laser Induced Damage Threshold14Local Structure Manipulates Nonlinear Optical Properties in Non-stoichiometric Lithium Niobate1Simple yet extraordinary: Super-polyhedra-built 3D chalcogenide framework of Cs5Ga9S16 with excellent infrared nonlinear optical performance29Regulation of Third‐Order NLO Properties by Central Metal Exchange of Heterogeneous MOFs@CeO221Characterizations and Nonlinear-Optical Properties of Pentanary Transition-Metal Oxysulfide Sr2CoGe2OS626High Quality and Large Size Yttrium Iron Garnet Crystal Grown by Top Seeded Solution Growth Technique10AIB3IIC3IIIQ8VI: A New Family for the Design of Infrared Nonlinear Optical Materials by Coupling Octahedra and Tetrahedra Units152AeMg6Ga6S16 (Ae = Ca, Sr, Ba): The First Double Alkaline‐Earth Metal Chalcogenides with Excellent Performances29Rb 2 CdSi 4 S 10 : novel [Si 4 S 10 ] T2-supertetrahedra-contained infrared nonlinear optical material with large band gap79Ag-based chalcogenides and derivatives as promising infrared nonlinear optical materials90Growth and characterization of IR nonlinear optical PbIn6Te10 crystal3Na 2 Ba[Na 2 Sn 2 S 7 ]: Structural Tolerance Factor‐Guided NLO Performance Improvement50Na2Ba[Na2Sn2S7]: Structural Tolerance Factor‐Guided NLO Performance Improvement0[Sr 4 Cl 2 ][Si 3 S 9 ]: Ultrawide-bandgap salt-inclusion thiosilicate nonlinear optical material with unprecedented tri-polymerized [Si 3 S 9 ] clusters21A 0.5 H 2 C 6 N 7 O 3 ·4H 2 O (A = Ca 2+ , Sr 2+ ) iso-cyamelurates with ultra-large π-conjugated group and excellent nonlinear optical properties10A new infrared nonlinear optical material BaZnGeS 4 with a wide band gap and large nonlinear optical response34Honeycomb layered topology construction for exceptional long-wave infrared nonlinear optical crystals29LaAeAl 3 S 7 (Ae = Ca, Sr): Cairo pentagonal layered thioaluminates achieving a good balance between a strong second harmonic generation response and a wide bandgap23Recent progress on sulfide infrared nonlinear optical materials with large SHG response and wide band gap26Synthesis, structure and characterization of Cd 2 TeO 3 Cl 2 with unprecedented [Cd 2 O 6 Cl 4 ] octahedral dimers5Visualizing the alignment of lone pair electrons in La 3 AsS 5 Br 2 and La 5 As 2 S 9 Cl 3 to form an acentric or centrosymmetric structure10Growth and Optical Properties of Large-Sized NaVO2(IO3)2(H2O) Crystals for Second-Harmonic Generation Applications12Engineering charge-transfer interactions for red-emitting SrLa(Sc,Ga)O4:Ce3+ phosphor with improved thermal stability22Recent progress in the design of IR nonlinear optical materials by partial chemical substitution: Structural evolution and performance optimization133Rational Design of a Rare‐Earth Oxychalcogenide Nd3[Ga3O3S3][Ge2O7] with Superior Infrared Nonlinear Optical Performance64Partial substitution induced structural transformation and enhanced nonlinear optical properties of Na2GaxIn6-xSe10 (x = 3, 3.76)23The First UV Nonlinear Optical Selenite Material: Fluorination Control in CaYF(SeO 3 ) 2 and Y 3 F(SeO 3 ) 485The First UV Nonlinear Optical Selenite Material: Fluorination Control in CaYF(SeO3)2 and Y3F(SeO3)47Clamping effect driven design and fabrication of new infrared birefringent materials with large optical anisotropy45Zn2BS3Br: An Infrared Nonlinear Optical Material with Significant Dual-Property Enhancements Designed through a Template Grafting Strategy20Unveiling the Superior Optical Properties of Novel Melamine‐Based Nonlinear Optical Material with Strong Second‐Harmonic Generation and Giant Optical Anisotropy74Optimal Design of Mid-Infrared Nonlinear-Optical Crystals: From SrZnSnSe 4 to SrZnSiSe 422ε-La(IO3)3: A Polar Iodate with High Thermal Stability and a Large Second-Harmonic-Generation Response Obtained by a Supercritical Hydrothermal Method8Crystal Growth, Thermal Treatment, and Characterization of Nonlinear Optical Crystal LiGa0.5In0.5Se2 for Mid-infrared Applications8Inherent law of SHG and phase-matching in 0D NLO materials: Permutation tetra-coordinated groups2HgB2S4: A d10 Metal Thioborate with Giant Birefringence and Wide Band Gap31Three‐in‐One Strategy Constructing the First High‐Performance Nonlinear Optical Sulfide Crystallizing with the P43 Space Group27Recent advances in IR nonlinear optical chalcogenides with well-balanced comprehensive performance56Zn 2 HgP 2 S 8 : A Wide Bandgap Hg‐Based Infrared Nonlinear Optical Material with Large Second‐Harmonic Generation Response75Rational Design of Noncentrosymmetric Organic–Inorganic Hybrids with a π-Conjugated Pyridium-Type Cation for High Nonlinear-Optical Performance19Mixed Anionic Tetrahedra Guided Design of New Infrared Nonlinear Optical Material Cs 3 Ga 8 S 13 Cl with High Laser‐Induced Damage Threshold26A ll HgM IV S 4 (A ll = Sr, Ba, M IV = Si, Ge): A Series of Materials with Large Second Harmonic Generation Response and Wide Band Gaps27Double alkaline earth metals sulfide SrMgGeS4 with high laser-induced damage threshold and strong second-harmonic generation29Theoretical investigations on ternary defective diamond-like infrared nonlinear optical materials in Be-Ga-Se system18Breaking Through the Trade‐Off Between Wide Band Gap and Large SHG Coefficient in Mercury‐Based Chalcogenides for IR Nonlinear Optical Application49Regulating the key performance parameters for Hg-based IR NLO chalcogenides via bandgap engineering strategy26Ga-based IR nonlinear optical materials: Synthesis, structures, and properties65“Three‐in‐One”: A New Hg‐Based Selenide Hg 7 P 2 Se 12 Exhibiting Wide Infrared Transparency Range and Strong Nonlinear Optical Effect80A UV non-hydrogen pure selenite nonlinear optical material for achieving balanced properties through framework-optimized structural transformation41Chemical modulation of A I RE III C IV QVI4 family compounds for band gap and optical anisotropy enhancement16Heteroanionic [VO x S 4− x ] groups: tetrahedral units with large birefringence for mid-infrared nonlinear optical crystals9Rare-earth-based chalcogenides and their derivatives: an encouraging IR nonlinear optical material candidate70Structural strategy for advancing nonlinear optical effects in 1D-[MX 2 ] ∞ chains: internal distortion and atomic types2Wide band gap selenide infrared nonlinear optical materials A II Mg 6 Ga 6 Se 16 with strong SHG responses and high laser-induced damage thresholds31Polysulfide Anions [S x ] 2− ( x = 2, 3, 4, 5): Promising Functional Building Units for Infrared Nonlinear Optical Materials22Advances, optical and electronic applications of functional materials based on rare earth sulfide semiconductors25Cs 3 In(In 4 Se 7 )(P 2 Se 6 ): A Multi‐Chromophore Chalcogenide with Excellent Nonlinear Optical Property Designed by Group Grafting55Cs3In(In4Se7)(P2Se6): A Multi‐Chromophore Chalcogenide with Excellent Nonlinear Optical Property Designed by Group Grafting2Hg3Se(SeO3)(SO4): A Mixed-Valent Selenium Compound with Mid-Infrared Transmittance Obtained by In Situ Reaction26UV-Transparent SHG Material Explored in an Alkali Metal Sulfate Selenite System16Evaluation and prospect of Mid-Infrared nonlinear optical materials in f0 rare earth (RE = Sc, Y, La) chalcogenides44[Na2PbI][Ga7S12]: Combining Diamond-Like Anionic Framework with Polycationic Chain toward Achieving Remarkable Nonlinear Optical Response21Mixed Anionic M(S/X)6 Polyhedra as Symmetry-Breaking Motifs to Enhance the Infrared Nonlinear Optical Response in Y–M–S–X (M = Ga, Ge; X = Cl, Br)5LaMg6Ga6S16: a chemical stable divalent lanthanide chalcogenide70The first Hg-based oxychalcogenide Sr2HgGe2OS6: Achieving balanced IR nonlinear optical properties through synergistic cation and anion substitution28A Rare Earth Chalcogenide Nonlinear Optical Crystal KLaGeS4: Achieving Good Balance among Band Gap, Second Harmonic Generation Effect, and Birefringence12Structure‐Prediction‐Oriented Synthesis of Thiophosphates as Promising Infrared Nonlinear Optical Materials24Structure‐Prediction‐Oriented Synthesis of Thiophosphates as Promising Infrared Nonlinear Optical Materials1Recent advances and future perspectives on rare-earth-based nonlinear optical materials with π-conjugated [XO3] (X = B, C, N) units66Ag 2 GeS 3 : A Diamond‐Like Chalcogenide as an IR Nonlinear Optical Material with Outstanding Second‐Harmonic Generation Response28Effects of different groups on phase-matching and SHG in “3+4” Pn materials0LaAgSiS4: Increasing Optical Birefringence in Rare Earth Chalcogenide by Addition of Planar [AgS3] Groups5Hg4InS2Cl5: Achieving Giant Optical Anisotropy by Introducing Well‐Aligned Linear [Hg2S2] Units14Emergent Mid‐Infrared Nonlinear Optical Candidates With Targeted Balance Performances17Rare‐Earth Substitution Induced Symmetry Breaking for The First Sc‐Based Nonlinear Optical Chalcogenide with High‐Performance303Pb 8 O 7 I 2 ·2CsI: the salt-inclusion strategy enriches the structural chemistry in lead oxyhalides1A wide band gap selenohalide Cs 9 Si 8 Se 20 Cl with unprecedented [CsSe 7 Cl] mixed anionic units2Isovalent cation substitution drives structural transformation and infrared nonlinear optical activity in Eu-based chalcogenides11NaCaGa 3 S 6 : a mixed alkali metal and alkaline earth metal sulfide with a distinctive [Ga 5 S 10 ] ∞ layered framework0Prismatic crystal field stabilized divalent rare-earth chalcogenide REIIBII6CIII6QVI16 with bifunctionality30磷属红外非线性光学晶体带隙调控的可能策略（特邀）5AI2Mg3Ga12S22 (AI = K, Rb): T2-type supertetrahedra coupled with [MgS6] octahedra for designing wide-band gap infrared nonlinear optical materials with well-balanced properties16Two-in-one: assembling hybrid supertetrahedra chromophores and achieving high-performance “hexagonal warriors” in nonlinear optical crystals6Chalcophosphates: A plentiful source of infrared nonlinear optical materials42Synergically Assembling Advantageous Groups toward High‐Performance Infrared Nonlinear Optical Materials A II CdSiSe 4 (A II = Sr, Ba)40AI4NLO: An Integrated Data Platform for Machine Learning-Driven Exploration of Inorganic Nonlinear Optical Materials8KYSiSe 4 : A Rare-Earth Selenide Infrared Nonlinear Optical Crystal with Wide Infrared Transparency and Well-Balanced E g and SHG Response9Nonlinear Optical Series A(VO2)3(SeO3)2 (A = NH4+, K+, and H3O+) with Large Birefringence Derived from High-Anisotropic VO6 Octahedra and SeO3 Pyramids8CaYIIIS 4 (III = Ga, In): Two Olivine-Type Compounds Exhibiting Exceptional Birefringence Properties1Inductive-Effect-Driven Tunability of Magnetism and Luminescence in Triangular Layers ANd(SO4)2 (A = Rb, Cs)0Reactive flux assisted metal oxide–boron–sulfur routine for syntheses of CsRESiS 4 (RE = Sm, Gd–Ho): featuring nonlinear optical activity and wide band gaps5ABCQ4型硫属化物红外非线性光学材料的构效关系（特邀）0LnMg 6 Ga 6 S 16 (Ln = Nd, Sm), two bifunctional optical materials exhibiting both nonlinear optical and photoluminescent properties0Polyhedral replacement-guided design of Ce3MnGaSe7 featuring strong second-harmonic genera-tion and high laser-induced damage threshold0Research on an Optical Crystal Detection Model Designed for Transmittance-Aware Analysis0van der Waals layered CuInP 2 S 6 as infrared nonlinear optical material1高性能硫属化物红外非线性光学材料构效关系（特邀）0Rare-Earth Selenophosphates Cs 2 YP 2 Se 7 and KYP 2 Se 6 Synthesized by the RFMOBQ Routine: Structural Evolution and Nonlinear Optical Activity2Growth and Enhancement of Magneto-Optical Properties in the Dysprosium-Doped Large-Size Yttrium Iron Garnet Crystal3KHg 4 Ga 5 S 12 : A Diamond-like Tetrahedral Chalcogenide Exhibiting Giant Phase-Matching Second Harmonic Generation6CdY 2 Si 2 S 8 : A Wide Bandgap IR NLO Material with d 10 Metal-Induced Structure Transformation from CS to NCS1The Power of Pnictogen Bond: As─As Linkages Drive Wide Bandgap, Strong NLO Response and Large Birefringence in SrGa 3 Si 4 As 115The Power of Pnictogen Bond: As─As Linkages Drive Wide Bandgap, Strong NLO Response and Large Birefringence in SrGa 3 Si 4 As 110Heterovalent Coexistence‐Driven Symmetry Breaking and Dimensional Evolution: Designing Polar Heart‐Shaped Channels for Exceptional MFIR Nonlinear Optics5Synthesis, structure, optical properties, and magnetic behavior of layered heavy rare-earth thiogermanates CsDyGeS4 and CsErGeS40d-f synergistic effect contributing record-high second-harmonic generation response in phase-matchable Mn-based chalcogenides0Variation of Tetrahedrons and Cations Regulates LIDTs in 3D‐DL Structure MIR‐NLO Crystals0

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  4. The Rise of Infrared Nonlinear Optical Pnictides: Advances and Outlooks

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  5. Synthesis, Crystal Structure, and Nonlinear Optical Property of an Anhydrous Sulfate KTb(SO4)2

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  34. Crystal Growth, Characterization, and Thermal Annealing of Nonlinear Optical Crystals AgGaGenSe2(n+1) (n = 1.5, 1.75, 2, 3, 4, 5, and 9) for Mid-infrared Applications

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  44. AIB3IIC3IIIQ8VI: A New Family for the Design of Infrared Nonlinear Optical Materials by Coupling Octahedra and Tetrahedra Units

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  45. AeMg6Ga6S16 (Ae = Ca, Sr, Ba): The First Double Alkaline‐Earth Metal Chalcogenides with Excellent Performances

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  46. Rb 2 CdSi 4 S 10 : novel [Si 4 S 10 ] T2-supertetrahedra-contained infrared nonlinear optical material with large band gap

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  47. Ag-based chalcogenides and derivatives as promising infrared nonlinear optical materials

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  48. Growth and characterization of IR nonlinear optical PbIn6Te10 crystal

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  49. Na 2 Ba[Na 2 Sn 2 S 7 ]: Structural Tolerance Factor‐Guided NLO Performance Improvement

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