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RESEARCH PAPER · Accounts of Chemical Research · 2022

Chemistry, Structure, and Function of Lone Pairs in Extended Solids

Geneva Laurita, Ram Seshadri

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Chemistry, Structure, and Function of Lone Pairs in Extended SolidsOriginalHalogen regulation triggers structural transformation from centrosymmetric to noncentrosymmetric switches in tin phosphate halides Sn 2 PO 4 X (X = F, Cl)47Negative Thermal Expansion in Fluoroapatite Pb5(VO4)3F Enhanced by the Steric Effect of Pb2+3Solution-Grown Ternary Semiconductors: Nanostructuring and Stereoelectronic Lone Pair Distortions in I–V–VI 2 Materials27Modification of CuSbS2 Photovoltaic Absorbent Properties via Defect Substitution0Stereochemically Active Lone Pairs and Nonlinear Optical Properties of Two-Dimensional Multilayered Tin and Germanium Iodide Perovskites116Thermoelectric materials13Vacancy-Driven Disorder and Elevated Dielectric Response in the Pyrochlore Pb1.5Nb2O6.57Metavalent Bonding Origins of Unusual Properties of Group IV Chalcogenides58Designing two-dimensional ferroelectric materials from phosphorus-analogue structures10Broadband emission originating from the stereochemical expression of 6s 2 lone pairs in two-dimensional lead bromide perovskites11Lone-pair, electron-dominated, nonlinear optical responses in sulfur clusters and electric tunability properties11Achieving Near‐unity Photoluminescence Quantum Yields in Organic‐Inorganic Hybrid Antimony (III) Chlorides with the [SbCl 5 ] Geometry129Achieving Near‐unity Photoluminescence Quantum Yields in Organic‐Inorganic Hybrid Antimony (III) Chlorides with the [SbCl5] Geometry16Effect of Hydrostatic Pressure on Lone Pair Activity and Phonon Transport in Bi2O2S11Lone Pair Rotation and Bond Heterogeneity Leading to Ultralow Thermal Conductivity in Aikinite51Boosting the CO2 adsorption performance by defect-rich hierarchical porous Mg-MOF-74126Effect of Stereochemically Active Electron Lone Pairs on Magnetic Ordering in Trivanadates8Toggling Stereochemical Activity through Interstitial Positioning of Cations between 2D V2O5 Double Layers12Tunable W5+ Absorbance in Laser Floating Zone Grown Bismuth Tungstate1Dynamic Lone Pairs and Fluoride-Ion Disorder in Cubic-BaSnF 431Synthesis and characterization of Sn-based electrolytes for F-ion batteries0Impact of Chiral Symmetry Breaking on Spin-Texture and Lone Pair Expression in Chiral Crystals of Hybrid Antimony and Bismuth Halides31In/Bi-based Direct- and Indirect-Gap Hybrid Double-Perovskite-Derived 1D Halides with Near-Unity Quantum Yield via Sb 3+ Doping34Metavalent Bonding in 2D Chalcogenides: Structural Origin and Chemical Mechanisms2Metavalent Bonding in 2D Chalcogenides: Structural Origin and Chemical Mechanisms17Hybrid Iodide Perovskites of Divalent Alkaline Earth and Lanthanide Elements16Rattling vibrations and occupied antibonding states yield intrinsically low thermal conductivity of the Zintl-phase compound KSrBi26Optical bandgap anomaly with tuning dimensionality in germanium perovskites: Interplay between quantum confinement and lone pair expression22Band engineering of layered oxyhalide photocatalysts for visible-light water splitting42Development and investigation of transition metal oxides having controllable ferroic properties0Hidden structures: a driving factor to achieve low thermal conductivity and high thermoelectric performance72Point-defect chemistry for ionic conduction in solid electrolytes with isovalent cation mixing16Toxic, radioactive, and disordered: a total scattering study of TlTcO 44Stereochemically Active Lone Pairs: Unraveling the Electronic Origin of Dielectric Response in Nonlinear Optical TeO211Screening Aluminum-Based Compounds as Low-κ Dielectrics for High-Frequency Applications17Manipulating Phase Transition and Ferroelectricity via Enhancing the Stereochemical Activity of Lone-Pair Electrons6On the limits of Zn doping in dual-polyhedral Cs7Cd3Br130Thermally Induced Lattice-Defective Oxygen Breathing in Perovskite-Structure Stannates with High-Contrast Reversible Thermochromism11Noncentrosymmetric Triangular Magnet CaMnTeO6: Strong Quantum Fluctuations and Role of s0 versus s2 Electronic States in Competing Exchange Interactions5Stability, Chemical Bonding, and Electron Lone Pair Localization in AsN at High Pressure by Density Functional Theory Calculations3A Lead‐Free Ferroelectric 2D Dion–Jacobson Tin Iodide Perovskite35Lone-Pair Origins of Polymorphism: Sn Monochalcogenides as a Case Study15Stereo‐Active Lone Pairs Induced Second Harmonic Generation Responses and Electrocatalytic Activity in Hybrid Material1Quantifying Structural Polarization by Continuous Regulation of Lone-Pair Electron Expression in Molecular Crystals52Graphene Oxide Covalently Functionalized with 5-Methyl-1,3,4-thiadiazol-2-amine for pH-Sensitive Ga3+ Recovery in Aqueous Solutions7Evidence of Lone Pair Crafted Emphanisis in the Ruddlesden–Popper Halide Perovskite Cs 2 PbI 2 Cl 219Dynamic Local Symmetry Fluctuations of Electron Density in Halide Perovskites15MnRhBi3: A Cleavable Antiferromagnetic Metal1Insights into Thermal Conductivity of Pnictogen Chalcogenides: Machine Learning Stereochemically Active Lone Pairs and Hybridization11Cooperative Regulation of n s 2 Lone-Pair Expression Realizes Distinct Excitonic Emissions in Hybrid Germanium, Tin, and Lead Halides27Diluting Ionic Liquids with Small Functional Molecules of Polypropylene Carbonate to Boost the Photovoltaic Performance of Perovskite Solar Cells3A novel zero-dimensional germanium-based ferroelectric hybrid material with dual phase transitions6First-principles investigation of lead-free Rb 3 SbX 6 (X = F, Cl, Br, I) mixed-halide double perovskites promising for photovoltaics and scintillation33Lone pair electron-induced attrition of lanthanide ions from a sillenite-structured bismuth gallate host2Stereochemical expression of Bi 6s 2 lone pairs mediates fluoride-ion (De)insertion in tunnel-structured Bi 2 PdO 4 and Bi 1.6 Pb 0.4 PtO 49Synthesis and large crystal growth of a family of mixed-anionic methanesulfonate salts by anionic site-substitution: Na 5 (SO 3 CH 3 ) 4 (X) (X = BF 4 − , ClO 4 − , PF 6 − , I − )9Stereoactive Lone-Pair Manipulation for High Thermoelectric Performance of GeSe-Based Compounds10Design of organic crystals with lone pairs to study spin resonance and spin-lattice interactions3High-Dielectric 2D Bismuth Oxides with Large Bandgaps: The Role of 6s2 Lone Pair Hybridization6Visualizing lone pairs and quantifying their bonding in solids with tight-binding Wannier models from first principles1Exploiting chemical bonding principles to design high-performance thermoelectric materials58Pressure-Induced Conglomerate to Racemate Transformation in a One-Dimensional Disulfide-Based Lead Halide6Lone Pair Electron Manipulation: A Promising Avenue for Tuning Properties in Functional Materials3Ferroelectric Rattling Enhances Thermoelectric Efficiency by Suppressing Thermal Transport in Metal Thio- and Selenophosphate Monolayers4The Dugganite Structure as a Host for New Colored Compounds and for Oxygen Evolution Studies1Alkali-metal (ammonium) cadmium hydroselenite halides: an interplay of two stoichiometries2Interplay Between Lone Pair Stereochemical Activity and Structural Anisotropy Drives Ultralow Thermal Conductivity in Layered AGeS 3 (A = Pb, Sn) Metal Sulfides10A Family of Luminescent Halido Cadmates with Bifunctional Diammonium Cations0Symmetry-Breaking Amplifies Lone Pair Expression and Orbital Splitting for Promising Chain-Like Thermoelectrics35A strategy to achieve giant optical anisotropy via integrating linear pseudohalogen and stereochemical active lone pair cation6The Role of Lone Pairs in Fast Oxide Ion Conduction in Rhombohedral Bi 0.8 Pr 0.2 O 1.54Covalency and Lone Pair-Driven Distortions in Sulfur-Doped Tin Niobate2The nature of defect tolerance in (some) halide perovskites5Melt-blown polypropylene with long chain branching characteristics was prepared by γ-radiation and melt blending1Diversified Synthesis of 0D Hybrid Indium Halides Crystal Structure and PLQY Enhancement via Solvent Environment Regulation and Sb 3+ Doping8High-Pressure Synthesis of Pnictogen Nitrides2Antibonding States Drive Anharmonicity and Low Thermal Conductivity in Edge-Sharing Metal Chalcogenides4Modulation of the Electronic and Vibrational Landscape in Lead Organic Chalcogenides0Photocatalytic CO 2 Reduction by Ternary Heterostructures of Sb 2 VO 5 Nanorods, CdS Quantum Dots, and a Zinc(II) Porphyrin Complex18Tailoring optical and ferroelectric properties in Sb 1− x Bi x SI van der Waals chalcohalides towards solar absorber applications4Unravelling lone pair induced bonding effects on thermal conductivity in metal chalcogenides using machine learning potentials2The Predictive Power of Chemical Bonding Analysis in Materials: A Perspective on Optoelectronic Properties4Inorganic Ge-based ferroelectric perovskites towards quasi-phase-matching in the infrared region0Large thermoelectric effect driven by high-order anharmonicity from synergistic lone-pair electrons and rattling modes in K 3 Au 3 Sb 20Non-isovalent substitution drives cooperative charge redistribution and enhanced dielectric screening in chalcogenides0Noncentrosymmetric hybrid gallium halides built from non-polar inorganic units3Theoretical exploration of As-based mixed halide double perovskites A 3 AsI 6 (A = K, Rb, and Cs) for photovoltaics applications using a DFT approach1Localized 2D/3D heterojunction enhances photovoltage for perovskite-organic tandem solar cells11Vibronic coupling-driven, environmentally stable, and optically efficient red light-emitting lead-free perovskite-inspired materials for color-converting devices1Cu 7.62 Bi 6 Se 12 Cl 6 I: Discovery of a Low Band Gap, Low Thermal Conductivity Mixed-Anion Material0Bulk crystal growth, physicochemical, and optical analysis of third-order nonlinear optical active 2-methylimidazolium hydrogen fumarate for optical limiting applications0Tuning the Phase Structure and Electrical Properties of BNKT‐Based Ceramics via Li + Doping0Stress-induced orbital splitting and lone-pair modulation in anharmonic phonon transport of BiAgSeO superlattice8Octahedral tilting and B-site off-centering in halide perovskites are not coupled7Lacunary lead apatite Pb6Ca2K2(PO4)6: multi-methodological structural investigation, optical and dielectric properties0Contrasting Lone-Pair Stereochemistry in Sb 3+ and Bi 3+ Chalcogenides: Implications for Structure and Phonon Transport2Enabling Record‐Low Coercive Field and Large Polarization in Hybrid Germanium Iodide Ferroelectric Through Chemical Bonding Engineering1Enabling Record‐Low Coercive Field and Large Polarization in Hybrid Germanium Iodide Ferroelectric Through Chemical Bonding Engineering1Ferroelastic phase transition in lead bismuth borate, PbBiOBO30An Atom-Precise Approach to Damp First-Order Phase Transitions and Its Implications for Neuromorphic Signal Processing1Antibonding Lone Pairs as Hidden Drivers of Bonding, Dynamics, and Energy Performance0Combining Anisotropic 119 Sn NMR and Ab Initio Calculations to Probe the Stereoactive Lone Pair in Sn(II) Metal–Organic Frameworks0Direct Observation of Noncollinear Ferrielectricity in a Two-Dimensional Hybrid Germanium Perovskite1Cs 2 M BiCl 6 ( M = Na , Ag) double perovskites: Emphanisis-driven charge carrier dynamics and piezoelectricity for their application as nanocomposites in mechanical energy harvesting0Structure–property relationships in novel quaternary Cs–Cu chalcogenides: A first-principles investigation for energy conversion applications0Cosine Bands, Flat Bands and Superconductivity in Orthorhombic Iron Selenide0Fluoride ions as charge carriers in electrochemical energy storage0Stereochemically Active Lone Electron Pairs in the Chalcogen Oxide-Carbonates Te[CO3]O and Te4O7[CO3] at Elevated Pressures0Insights into the catalytic removal of diclofenac in water by zinc in the presence of Co3O4, Co(OH)2 and Ni(OH)2: Performance and mechanism1Metal-organic framework-based mercury detection sensors: From recognition and enrichment to signal output0Unlock lasing in two-dimensional metal halide perovskites by tuning ns 2 lone pairs2Native Defects‐Induced Fermi‐Level Pinning and Diffuson‐Mediated Thermal Transport in BiSbSe 3 Thermoelectrics0Structural Origins of Forbidden Emission in Two-Dimensional Lead Halide Perovskites0Pressure-Induced Interlayer Bonding in Arsenic Revealed by Single-Crystal Synchrotron X-ray Diffraction in a Diamond Anvil Cell0Melting Point Depression and Glass-Forming Abilities in Pb- and Sn-Based Hybrid Perovskites with a Nonprimary Ammonium Cation0Mixed-Anion Mischief: Lone Pairs Meet Ionic Bonds to Suppress Thermal Transport in Quasi-1D Bi3Se4Br0

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  2. Negative Thermal Expansion in Fluoroapatite Pb5(VO4)3F Enhanced by the Steric Effect of Pb2+

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  3. Solution-Grown Ternary Semiconductors: Nanostructuring and Stereoelectronic Lone Pair Distortions in I–V–VI 2 Materials

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  4. Modification of CuSbS2 Photovoltaic Absorbent Properties via Defect Substitution

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  15. Lone Pair Rotation and Bond Heterogeneity Leading to Ultralow Thermal Conductivity in Aikinite

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  33. Toxic, radioactive, and disordered: a total scattering study of TlTcO 4

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  43. Stereo‐Active Lone Pairs Induced Second Harmonic Generation Responses and Electrocatalytic Activity in Hybrid Material

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  44. Quantifying Structural Polarization by Continuous Regulation of Lone-Pair Electron Expression in Molecular Crystals

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  45. Graphene Oxide Covalently Functionalized with 5-Methyl-1,3,4-thiadiazol-2-amine for pH-Sensitive Ga3+ Recovery in Aqueous Solutions

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  46. Evidence of Lone Pair Crafted Emphanisis in the Ruddlesden–Popper Halide Perovskite Cs 2 PbI 2 Cl 2

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  47. Dynamic Local Symmetry Fluctuations of Electron Density in Halide Perovskites

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  48. MnRhBi3: A Cleavable Antiferromagnetic Metal

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    Eleanor M. Clements, Dmitry Ovchinnikov, Parul R. Raghuvanshi, Valentino R. Cooper, Satoshi Okamoto, Andrew D Christianson, Joseph A. M. Paddison, Brenden R. Ortiz, Stuart Calder, Andrew F. May, Xiaodong Xu, Jiaqiang Yan, Michael A. McGuire

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  49. Insights into Thermal Conductivity of Pnictogen Chalcogenides: Machine Learning Stereochemically Active Lone Pairs and Hybridization

    Chemistry of Materials · 2024-12-13

    Harpriya Minhas, Milan Kumar Jena, Rahul Kumar Sharma, Biswarup Pathak

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  50. Cooperative Regulation of n s 2 Lone-Pair Expression Realizes Distinct Excitonic Emissions in Hybrid Germanium, Tin, and Lead Halides

    Journal of the American Chemical Society · 2024-12-17

    Han Jiang, Yawen Li, Peijie Zhang, Bin Xu, Xiaofan Xu, Zewei Quan

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