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RESEARCH PAPER · ACS Materials Letters · 2022

RbBiP2S6: A Promising IR Nonlinear Optical Material with a Giant Second-Harmonic Generation Response Designed by Aliovalent Substitution

Man-Man Chen, Shenghua Zhou, Wenbo Wei, Mao‐Yin Ran, Bingxuan Li, Xintao Wu, Hua Lin, Qi‐Long Zhu

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RbBiP2S6: A Promising IR Nonlinear Optical Material with a Giant Second-Harmonic Generation Response Designed by Aliovalent SubstitutionOriginalBridging oxygen atoms in trigonal prism units driven strong second-harmonic-generation efficiency in Sr 3 Ge 2 O 4 Te 318Interesting dimensional transition through changing cations as the trigger in multinary thioarsenates displaying variable photocurrent response and optical anisotropy22Phase matching achieved by isomorphous substitution in IR nonlinear optical material Ba 2 SnSSi 2 O 7 with an undiscovered [SnO 4 S] functional motif47Rational design via dual-site aliovalent substitution leads to an outstanding IR nonlinear optical material with well-balanced comprehensive properties68The exploration of new infrared nonlinear optical crystals based on the polymorphism of BaGa 4 S 731A comprehensive review on metal chalcogenides with three-dimensional frameworks for infrared nonlinear optical applications114Oxychalcogenides as Promising Ultraviolet Nonlinear Optical Candidates: Experimental and Theoretical Studies of AEGeOS2(AE = Sr and Ba)24Simple yet extraordinary: Super-polyhedra-built 3D chalcogenide framework of Cs5Ga9S16 with excellent infrared nonlinear optical performance29A review of structures and physical properties of rare earth chalcophosphates77Synthesis, Crystal and Electronic Structures, Nonlinear Optical Properties, and Magnetic Properties of Two Thiophosphates: KInP2S7 and KCrP2S79KREP2Se6 (RE = Sm, Gd, Tb): The First Rare‐Earth Selenophosphates with Remarkable Nonlinear Optical Activities Realized by Synergistic Effect of RE‐ and P‐Based Motifs39Ba5Ga2SiO4S6: a Phase-Matching Nonlinear Optical Oxychalcogenide Design via Structural Regulation Originated from Heteroanion Introduction25γ-P 4 S 3 I 2 : a new metal-free infrared second-order nonlinear optical crystal designed by polymorphism strategy17Na 2 Ba[Na 2 Sn 2 S 7 ]: Structural Tolerance Factor‐Guided NLO Performance Improvement50Na2Ba[Na2Sn2S7]: Structural Tolerance Factor‐Guided NLO Performance Improvement0A novel bifunctional thioarsenate based on unprecedented molecular [Cd 4 As 8 Se 16 (Se 2 ) 2 ] 8− cluster anions11A unique [Sb 6 O 2 S 13 ] 12− finite chain in oxychalcogenide Ba 6 Sb 6 O 2 S 13 leading to ultra-low thermal conductivity and giant birefringence12An overview of Mg-based IR nonlinear optical materials22Heteroanion-introduction-driven birefringence enhancement in oxychalcogenide Ba 3 M II Ge 3 O 2 S 8 (M II = Mn, Cd)19Melilite oxychalcogenide Sr 2 FeGe 2 OS 6 : a phase-matching IR nonlinear optical material realized by isomorphous substitution30Recent advances in F-containing iodate nonlinear optical materials6Revisiting 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 response12LnLiSiS4 (Ln = La and Ce): Promising infrared nonlinear optical materials designed by aliovalent substitution from SrCdSiS437Rational Design of a Rare‐Earth Oxychalcogenide Nd3[Ga3O3S3][Ge2O7] with Superior Infrared Nonlinear Optical Performance64Y3Fe0.5SiSe7: A new cation-deficient quaternary mixed transition metal chalcogenide with extremely low thermal conductivity3{[In2S7]8–}∞ Chain and Isolated HgS4 Planar Unit Constructed One-Dimensional Pentanary Sulfide K2Ba7HgIn4S16 Exhibiting Nonlinear-Optical Activity10Recent advances in IR nonlinear optical chalcogenides with well-balanced comprehensive performance56Cd2Nb2Te4O15: A Novel Pseudo‐Aurivillius‐Type Tellurite with Unprecedented Nonlinear Optical Properties and Excellent Stability40AEAg7(PS4)3 (AE = Ba, Sr): The homovalent substitution of lead by alkaline earth metals achieves the separation of the two phases and enlarges the band gap1Two Noncentrosymmetric Bismuth Phosphates: Rational Design Synthesis and Optical Properties4LiGa(IO3)4: An Excellent NLO Material with Unprecedented 2D [Ga(IO3)4]∞− Layer Synthesized by Aliovalent Substitution20Double alkaline earth metals sulfide SrMgGeS4 with high laser-induced damage threshold and strong second-harmonic generation29Breaking Through the Trade‐Off Between Wide Band Gap and Large SHG Coefficient in Mercury‐Based Chalcogenides for IR Nonlinear Optical Application49Noncentrosymmetric Na6Pb3P4S16 and Centrosymmetric K2MIIP2S6 (MII = Mg and Zn) Displaying Multiple Membered-Ring Configurations and Strong Optical Anisotropy10Regulating the key performance parameters for Hg-based IR NLO chalcogenides via bandgap engineering strategy26ACu4AsS4 (A = K, Rb): Two infrared nonlinear optical crystals with strong second-harmonic generation responses originating from multiple chromophores12Ga-based IR nonlinear optical materials: Synthesis, structures, and properties65Ba 2 GeF 2 Q 3 (Q = S, Se) and Ba 3 GeF 2 Se 4 : new F-based chalcohalides with enhanced birefringence9Chalcophosphate metasurfaces with multipolar resonances and electro-optic tuning7Hydrothermally synthesized first acentric apatite (Bi 5 Na 5 )[PO 4 ] 6 Cl 2 with wide Bi–Na isomorphism and doubled c -axis3Rare-earth-based chalcogenides and their derivatives: an encouraging IR nonlinear optical material candidate70RbPbPS 4 : a promising IR nonlinear optical material achieved by lone-pair-cation-substitution-induced structure transformation23Infrared nonlinear optical materials with multiple strongly ionic cations5The first Hg-based oxychalcogenide Sr2HgGe2OS6: Achieving balanced IR nonlinear optical properties through synergistic cation and anion substitution28Influence of Cation-Size Effects of Alkaline Earth (Ae) Metals on Dimensionality and Optical Anisotropy Regulation in K4AeP2S8 Thiophosphates5PbBeB2O5: A High-Performance Ultraviolet Nonlinear-Optical Crystal with Functional [BeB2O8]8– Group3Homoatomic Polychalcogenide Nonlinear Optical Anionic Groups with Ultra-Large Optical Anisotropy31Recent 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 Response28The centrosymmetric to non-centrosymmetric transformation induced by alkaline-earth cations producing infrared nonlinear optical AeMn6Ga6S16 (Ae = Ca, Sr)13β-Pb3P2S8: A new optical crystal with exceptional birefringence effect11Realizing Excellent Infrared Nonlinear Optical Performance in Eu-Based Chalcogenides via Rational Cross Substitution Strategy26ACuGa 6 S 10 (A = Rb, Cs): Design and Synthesis of Two New Cavity‐Chalcopyrite Chalcogenides Based on “Iterative Substitution” Strategy4From [Ba3S][GeS4] to [Ba3CO3][MS4] (M = Ge, Sn): Enhancing optical anisotropy in IR birefringent crystals via functional group implantation11Balanced IR Nonlinear Optical Performance Achieved by Cation–Anion Module Cosubstitution in V-Based Salt-Inclusion Oxychalcogenides22Exploring new horizons in mid-to-far infrared nonlinear optical crystals: the significant potential of trigonal pyramidal [TeS 3 ] 2− functional units18Isovalent cation substitution drives structural transformation and infrared nonlinear optical activity in Eu-based chalcogenides11Phase transition engineering to break the symmetry of diamond-like chalcogenide for second-order nonlinear optics2Ionothermal syntheses, structures, and photocurrent responses of two-dimensional layered thiostannates1Symmetry over Chemistry: Harmonic Generation of Low-Dimensional Alkali Chalcopnictates RbMP2S6 (M = Sb, Bi)5Recent progress in structural design strategies of high-birefringence optical crystals54The Influence of Different Group Distortions on the Structure–Property Relationship of Alkali Metal Thiophosphate0Alkali Metal Substitution-Induced Structural Transformation for RbREP2Se6 (RE = Gd, Tb, Dy) with Second-Harmonic Generation Responses6Synergistic Enhancement of Band Gap and Optical Anisotropy via Functional-Site Cosubstitution in Antiperovskite-Type Chalcohalides [Ba2K][X][MS4] (M = Ge, Si; X = Cl, Br)2Structure-property relationships in IR nonlinear optical chalcogenides with stereochemically active lone pairs29Vacancy-driven tetrahedral distortion leading to exceptional second harmonic generation3A high-performance IR nonlinear optical material Sr 3 MnGe 2 S 8 achieved via partial cation substitution-induced structural transformation2Maximizing the second-harmonic generation response via coordination-induced localization of nonbonding electrons12ANb 2 (PS 4 )(S 2 ) 3 (A = K, Rb, Cs): the first Nb-based NLO thiophosphates with [NbS 2 (S 2 ) 3 ] and [Nb 2 PS 6 (S 2 ) 4 ] units exhibiting tri-state structural transformation and high performance6Charge-order-induced directional enhancement of non-diagonal second-order nonlinear optical tensor components2Optimal three-dimensional [Ag 4 P 2 S 6 ]-framework assembly directed by a threefold roto-inversion axis for enhanced birefringence0van der Waals layered CuInP 2 S 6 as infrared nonlinear optical material1Rare-Earth Selenophosphates Cs 2 YP 2 Se 7 and KYP 2 Se 6 Synthesized by the RFMOBQ Routine: Structural Evolution and Nonlinear Optical Activity2KHg 4 Ga 5 S 12 : A Diamond-like Tetrahedral Chalcogenide Exhibiting Giant Phase-Matching Second Harmonic Generation6[Ba2K][Br][SiS4]: An antiperovskite-type chalcohalide with simultaneously enhanced birefringence and band gap via cation-anion co-substitution0Circumventing the Eg–SHG trade-off in selenides: Salt-inclusion [X4Br2][MGa4Se10] with concurrent large band gap and strong nonlinear optical response1Mineral‐Inspired and Computation‐Assisted Rational Design of Polar Gittinsite‐Type Thiophosphates With Exceptional Nonlinear Optical Performance3AVP2S7 (A = K, Rb): Dual-Optimized Infrared Nonlinear Optical Thiophosphates via Heterovalent-Substitution-Driven Symmetry Breaking and Reinforced Interlayer Interactions0Laporte Selection Rule Induced the Suppression of d ‐ d Transitions and Vacancies Enhanced the Second Harmonic Generation in I 4¯‐MnGa 2 S 40Domino‐Effect Amplification via Covalent‐Chain Engineering for Giant Birefringence in NaAsQ 2 (Q = S, Se) Crystals0

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  2. Interesting dimensional transition through changing cations as the trigger in multinary thioarsenates displaying variable photocurrent response and optical anisotropy

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  3. Phase matching achieved by isomorphous substitution in IR nonlinear optical material Ba 2 SnSSi 2 O 7 with an undiscovered [SnO 4 S] functional motif

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  4. Rational design via dual-site aliovalent substitution leads to an outstanding IR nonlinear optical material with well-balanced comprehensive properties

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  7. Oxychalcogenides as Promising Ultraviolet Nonlinear Optical Candidates: Experimental and Theoretical Studies of AEGeOS2(AE = Sr and Ba)

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  8. Simple yet extraordinary: Super-polyhedra-built 3D chalcogenide framework of Cs5Ga9S16 with excellent infrared nonlinear optical performance

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  13. γ-P 4 S 3 I 2 : a new metal-free infrared second-order nonlinear optical crystal designed by polymorphism strategy

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

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  16. A novel bifunctional thioarsenate based on unprecedented molecular [Cd 4 As 8 Se 16 (Se 2 ) 2 ] 8− cluster anions

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  17. A unique [Sb 6 O 2 S 13 ] 12− finite chain in oxychalcogenide Ba 6 Sb 6 O 2 S 13 leading to ultra-low thermal conductivity and giant birefringence

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  19. Heteroanion-introduction-driven birefringence enhancement in oxychalcogenide Ba 3 M II Ge 3 O 2 S 8 (M II = Mn, Cd)

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  20. Melilite oxychalcogenide Sr 2 FeGe 2 OS 6 : a phase-matching IR nonlinear optical material realized by isomorphous substitution

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