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RESEARCH PAPER · Dalton Transactions · 2015

Understanding ferroelectricity in layered perovskites: new ideas and insights from theory and experiments

Nicole A. Benedek, James M. Rondinelli, Hania Djani, Philippe Ghosez, Philip Lightfoot

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Understanding ferroelectricity in layered perovskites: new ideas and insights from theory and experimentsOriginalCoupling and Electrical Control of Structural, Orbital and Magnetic Orders in Perovskites58Anharmonic lattice interactions in improper ferroelectrics for multiferroic design72Ferroelectricity from coupled cooperative Jahn-Teller distortions and octahedral rotations in ordered Ruddlesden-Popper manganates28ChemInform Abstract: Understanding Ferroelectricity in Layered Perovskites: New Ideas and Insights from Theory and Experiments0Coupling and electrical control of structural, orbital and magnetic orders in perovskites98Proper Ferroelectricity in the Dion–Jacobson Material CsBi2Ti2NbO10: Experiment and Theory56Recent advances in multiferroic oxide heterostructures and devices100Improper Inversion Symmetry Breaking and Piezoelectricity through Oxygen Octahedral Rotations in Layered Perovskite Family, LiRTiO4 (R = Rare Earths)34‘Ferroelectric’ metals reexamined: fundamental mechanisms and design considerations for new materials161Columnar shifts as symmetry-breaking degrees of freedom in molecular perovskites68Combined experimental and density functional theory studies of an organic–inorganic hybrid perovskite17Hybrid improper ferroelectricity in SrZrO 3 /BaZrO 3 superlattice9Importing spontaneous polarization into a Heisenberg ferromagnet for a potential single-phase multiferroic53Microscopic mechanistic study on the multiferroic of R 2 CoMnO 6 /La 2 CoMnO 6 (R = Ce, Pr, Nd, Pm, Sm, Gd, Tb, Dy, Ho, Er, Tm) by chemical and hydrostatic pressures: a first-principles calculation14NdBaScO 4 : aristotype of a new family of geometric ferroelectrics?16Spin texture induced by oxygen vacancies in strontium perovskite (001) surfaces: A theoretical comparison between SrTiO3 and SrHfO325Electric Field Control of Jahn-Teller Distortions in Bulk Perovskites64Controlling the cation distribution and electric polarization with epitaxial strain in Aurivillius-phase Bi5FeTi3O1513Designing New Improper Ferroelectrics with a General Strategy0Two New Non-centrosymmetric n = 3 Layered Dion–Jacobson Perovskites: Polar RbBi2Ti2NbO10 and Nonpolar CsBi2Ti2TaO1057An efficient ab-initio quasiharmonic approach for the thermodynamics of solids89Octahedral rotation patterns in strained EuFeO3 and otherPbnmperovskite films: Implications for hybrid improper ferroelectricity31La 2 SrCr 2 O 7 : Controlling the Tilting Distortions of n = 2 Ruddlesden–Popper Phases through A-Site Cation Order32Unusual Relaxor Ferroelectric Behavior in Stairlike Aurivillius Phases21Ferroelectric and magnetic properties in 85 nm-thick Bi6Fe2Ti3O18 thin films by a modified sol-gel processing2Mechanism of polarization switching in wurtzite-structured zinc oxide thin films61Tunable Negative Thermal Expansion in Layered Perovskites from Quasi-Two-Dimensional Vibrations46Domains and ferroelectric switching pathways in Ca 3 Ti 2 O 7 from first principles74Conductivity Analysis of Bi4Ti3O12 Ferroelectric Ceramic: A Comprehensive Study from the Dynamic Aspects of Hopping Conduction0Directed Lifting of Inversion Symmetry in Ruddlesden–Popper Oxide–Fluorides: Toward Ferroelectric and Multiferroic Behavior57The role of Tb-doping on the structural and functional properties of Bi4−xTbxTi3O12 ferroelectric phases with the Aurivillius type structure4First-principles reinvestigation of bulk WO 361Covalent and Ionic Functionalization of HLN Layered Perovskite by Sonochemical Methods7To superspace and beyond1Electronic, optical and thermoelectric properties of bulk and surface (001) CuInTe 2 : A first principles study24Designing new ferroelectrics with a general strategy112Ferroelectric properties of highly c -oriented epitaxial Bi 2 WO 6 thin films18Structural refinement of Pbnm-type perovskite films from analysis of half-order diffraction peaks39On the “alpha-phase” of Ca2−xSrxMnO4 and extending the chemistry of Sr7−yCayMn4O15 to y>13Polar Oxides without Inversion Symmetry through Vacancy and Chemical Order43Composition dependence of the multifunctional properties of Nd-doped Bi4Ti3O12 ceramics37Learning from data to design functional materials without inversion symmetry95Magnetic order in four-layered Aurivillus phases36Phase Transition Behavior of the Layered Perovskite CsBi0.6La0.4Nb2O7: A Hybrid Improper Ferroelectric12Atomic Layer Engineering of High-κ Ferroelectricity in 2D Perovskites83Structural Modification of the Cation-Ordered Ruddlesden–Popper Phase YSr2Mn2O7 by Cation Exchange and Anion Insertion19Designing of metallic nanocrystals embedded in non-stoichiometric perovskite nanomaterial and its surface-electronic characteristics22Electric-Magneto-Optical Kerr Effect in a Hybrid Organic–Inorganic Perovskite75First-principles study of tungsten trioxide: Structural properties and polaron formation0Magnetic and ferroelectric properties of Aurivillius phase Bi7Fe3Ti3O21 and their doped films19Theory and Neutrons Combine To Reveal a Family of Layered Perovskites without Inversion Symmetry47New Type of 2D Perovskites with Alternating Cations in the Interlayer Space, (C(NH 2 ) 3 )(CH 3 NH 3 ) n Pb n I 3 n +1 : Structure, Properties, and Photovoltaic Performance521Crystal Structure of Electroceramics0Nanoarchitectonics in dielectric/ferroelectric layered perovskites: from bulk 3D systems to 2D nanosheets62Momentum-resolved observations of the phonon instability driving geometric improper ferroelectricity in yttrium manganite38Evolution of structure and ferroelectricity in Aurivillius Bi 4 Bi n−3 Fe n−3 Ti 3 O 3n+3 thin films51FIRST-PRINCIPLES STUDIES OF FERROELECTRIC PROPERTIES IN ORGANIC CRYSTAL AND PEROVSKITE SUPERLATTICES0Insights into the polymorphism of Bi 2 W 2 O 9 : single crystal growth and a complete survey of the variable-temperature thermal and dielectric properties11Isosymmetric structural phase transition of the orthorhombic lanthanum gallate structure as a function of temperature determined by Rietveld analysis6Self-Assembled Barium Titanate Nanoscale Films by Molecular Beam Epitaxy0Soft chemistry of ion-exchangeable layered metal oxides183Soft antiphase tilt of oxygen octahedra in the hybrid improper multiferroic Ca3Mn1.9Ti0.1O732Structural analysis of LaVO3 thin films under epitaxial strain32Improper ferroelectric polarization in a perovskite driven by intersite charge transfer and ordering23Morphology effect on photocatalytic activity in Bi 3 Fe 0.5 Nb 1.5 O 910Realizing selective water splitting hydrogen/oxygen evolution on ferroelectric Bi3TiNbO9 nanosheets105Out-of-plane polarization in a layered manganese chloride hybrid17Recipes for improper ferroelectricity in molecular perovskites121Nonswitchable polarization and magnetoelectric coupling in the high-pressure synthesized doubly ordered perovskites NaYMnWO6 and NaHoCoWO636Magnetic and electronic properties of the ferroelectric-photovoltaic ordered double perovskite CaMnTi2O6 investigated by x-ray absorption spectroscopies12Complex octahedral tilt phases in the ferroelectric perovskite system LixNa1−xNbO315A group-theoretical approach to enumerating magnetoelectric and multiferroic couplings in perovskites39A symmetry roadmap to new perovskite multiferroics3Direct observation of ferroelectricity in Ca3Mn2O7 and its prominent light absorption81An algebraic approach to cooperative rotations in networks of interconnected rigid units34Direct Magnetization-Polarization Coupling in BaCuF431Structure Dependent Phase Stability and Thermal Expansion of Ruddlesden–Popper Strontium Titanates25Design of New Multiferroic Oxides1Control of Uniaxial Negative Thermal Expansion in Layered Perovskites by Tuning Layer Thickness22Hybrid Improper Ferroelectricity in (Sr,Ca) 3 Sn 2 O 7 and Beyond: Universal Relationship between Ferroelectric Transition Temperature and Tolerance Factor in n = 2 Ruddlesden–Popper Phases123Cation Exchange as a Mechanism To Engineer Polarity in Layered Perovskites33Lead-free A 2 Bi 4 Ti 5 O 18 thin film capacitors (A = Ba and Sr) with large energy storage density, high efficiency, and excellent thermal stability72A hybrid fluoride layered perovskite, ( en H 2 )MnF 410Bulk crystal growth and characterization of the bismuth ferrite-based material Bi 3 FeO 4 (MoO 4 ) 213Tuning octahedral tilts and the polar nature of A -site deficient perovskites3Polarization rotation in Bi4Ti3O12 by isovalent doping at the fluorite sublattice24Atomic and electronic structure of domains walls in a polar metal22Focus on the ferroelectric polarization behavior of four-layered Aurivillius multiferroic thin film23Magnetoelectricity in multiferroics: a theoretical perspective267Advances in magnetoelectric multiferroics1766Machine learning guided design of functional materials with targeted properties60Unexpected phase transition sequence in the ferroelectric Bi4Ti3O1219Tuning perovskite oxides by strain: Electronic structure, properties, and functions in (electro)catalysis and ferroelectricity290A Room‐Temperature Ferroelectric Ferromagnet in a 1D Tetrahedral Chain Network39Crystal structure, optical and electronic properties studies on an hybrid multifunctional MnCl4-based material10A -site cation size effect on oxygen octahedral rotations in acentric Ruddlesden-Popper alkali rare-earth titanates11Mapping the structural transitions controlled by the trilinear coupling in Ca3-xSrxTi2O717Deliberate Deficiencies: Expanding Electronic Function through Non-stoichiometry13Fabrication of bismuth titanate nanosheets with tunable crystal facets for photocatalytic degradation of antibiotic56Temperature-Induced Structural Transformations in Undoped and Eu3+-Doped Ruddlesden–Popper Phases Sr2SnO4 and Sr3Sn2O7: Relation to the Impedance and Luminescence Behaviors13Ferroelectric polarization and fatigue characterization in bismuth-based Aurivillius thin films at lower voltage11Hybrid-improper ferroelectric behavior in Ba3SiO/Ba3GeO oxide antiperovskite superlattices8Towards photoferroic materials by design: recent progress and perspectives17Rationalizing and engineering Rashba spin-splitting in ferroelectric oxides86Magneto-electric multiferroics: designing new materials from first-principles calculations10Phase transitions in Bi4Ti3O1211Crystal Engineering of Bi 2 WO 6 to Polar Aurivillius-Phase Oxyhalides28Infrared nano-spectroscopy of ferroelastic domain walls in hybrid improper ferroelectric Ca3Ti2O731Observation of oxygen pyramid tilting induced polarization rotation in strained BiFeO 3 thin film3Lattice dynamics of the hybrid improper ferroelectrics (Ca,Sr)3Ti2O79Cobalt-induced structural modulation in multiferroic Aurivillius-phase oxides25Structural variations in (001)-oriented layered lead halide perovskites, templated by 1,2,4-triazolium16Hidden improper ferroelectric phases for design of antiferroelectrics3Anion Ordered and Ferroelectric Ruddlesden–Popper Oxynitride Ca3Nb2N2O5 for Visible-Light-Active Photocatalysis28Magnetically driven phonon instability enables the metal–insulator transition in h-FeS32Bi2W2O9 : A potentially antiferroelectric Aurivillius phase14Synergistic Influence of d0 (Nb5+) and d10 (Cd2+) Cations in Stabilizing Noncentrosymmetric Dion–Jacobson Layered Perovskites, A′Cd2Nb3O10 (A′ = Rb, Cs)12Robust In‐Plane Ferroelectricity in Ultrathin Epitaxial Aurivillius Films45Electron-lattice interplay in LaMnO3 from canonical Jahn-Teller distortion notations34Synthesis of Bi4Ti3O12-BaTiO3 nanocomposite, manifesting high dielectric and unique magnetic nature applicable in heterogeneous photocatalytic activity for degradation of Rhodamine B dye19From first- to second-order phase transitions in hybrid improper ferroelectrics through entropy stabilization21Large Switchable Photoconduction within 2D Potential Well of a Layered Ferroelectric Heterostructure38Ab-initio investigation of optoelectronic and thermoelectric properties in new p-type Rattling Heuslers Sr2PtX (X=Se and Te)4Ferroelectricity of Dion–Jacobson layered perovskites CsNdNb 2 O 7 and RbNdNb 2 O 720Defect accommodation in off-stoichiometric (SrTiO3)nSrO Ruddlesden–Popper superlattices studied with positron annihilation spectroscopy13Structural Diversity in Layered Hybrid Perovskites, A2PbBr4 or AA′PbBr4, Templated by Small Disc-Shaped Amines39Exploring the A2BX3 Family for New Functional Materials Using Crystallographic Database Mining and First-Principles Calculations5Polar Structures of KNdNb2O7and KNdTa2O710Tuning between Proper and Hybrid-Improper Mechanisms for Polar Behavior in Cs Ln 2Ti2NbO10 Dion-Jacobson Phases22A Multiaxial Layered Halide Double Perovskite Ferroelectric with Multiple Ferroic Orders69Unraveling the Suppression of Oxygen Octahedra Rotations in A3B2O7 Ruddlesden-Popper Compounds: Engineering Multiferroicity and Beyond53Hybrid improper antiferroelectricity—New insights for novel device concepts2Multiferroic heterostructures for spintronics31Rational Assembly of Two-Dimensional Perovskite Nanosheets as Building Blocks for New Ferroelectrics21Unveiling the mechanisms behind the ferroelectric response in the Sr(Nb,Ta)O 2 N oxynitrides6Naturally Layered Aurivillius Phases: Flexible Scaffolds for the Design of Multiferroic Materials5Growth and Atomically Resolved Polarization Mapping of Ferroelectric Bi2WO6 Thin Films25Review on Recent Developments in 2D Ferroelectrics: Theories and Applications334Cooperative Nature of Ferroelectricity in Two-Dimensional Hybrid Organic–Inorganic Perovskites39Facile synthesis of efficient heterogeneous photocatalytic and highly dielectric Bi4BaTi4O15 ceramic with remarkable applicability in the degradation of rhodamine B dye4Switching between Proper and Hybrid-Improper Polar Structures via Cation Substitution in A2La(TaTi)O7(A = Li, Na)17Strong trilinear coupling of phonon instabilities drives the avalanche-like hybrid improper ferroelectric transition in SrBi2Nb2O92Ferroelectricity and multiferroicity in anti–Ruddlesden–Popper structures25Negative thermal expansion in the Ruddlesden-Popper calcium titanates18Ultra-thin ferroelectrics93Lattice assisted dielectric relaxation in four-layer Aurivillius Bi 5 FeTi 3 O 15 ceramic at low temperatures6Symmetry mode analysis of distorted polar/nonpolar structures in A -site ordered SmBaMn2O6 perovskite8Structural chemistry of layered lead halide perovskites containing single octahedral layers59Structural Features in Some Layered Hybrid Copper Chloride Perovskites: ACuCl4 or A2CuCl427Towards the robust hydrogen (H2) fuel production with niobium complexes-A review96

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  2. Anharmonic lattice interactions in improper ferroelectrics for multiferroic design

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  3. Ferroelectricity from coupled cooperative Jahn-Teller distortions and octahedral rotations in ordered Ruddlesden-Popper manganates

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  4. ChemInform Abstract: Understanding Ferroelectricity in Layered Perovskites: New Ideas and Insights from Theory and Experiments

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  5. Coupling and electrical control of structural, orbital and magnetic orders in perovskites

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  6. Proper Ferroelectricity in the Dion–Jacobson Material CsBi2Ti2NbO10: Experiment and Theory

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  8. Improper Inversion Symmetry Breaking and Piezoelectricity through Oxygen Octahedral Rotations in Layered Perovskite Family, LiRTiO4 (R = Rare Earths)

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  9. ‘Ferroelectric’ metals reexamined: fundamental mechanisms and design considerations for new materials

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  14. Microscopic mechanistic study on the multiferroic of R 2 CoMnO 6 /La 2 CoMnO 6 (R = Ce, Pr, Nd, Pm, Sm, Gd, Tb, Dy, Ho, Er, Tm) by chemical and hydrostatic pressures: a first-principles calculation

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  15. NdBaScO 4 : aristotype of a new family of geometric ferroelectrics?

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  16. Spin texture induced by oxygen vacancies in strontium perovskite (001) surfaces: A theoretical comparison between SrTiO3 and SrHfO3

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  17. Electric Field Control of Jahn-Teller Distortions in Bulk Perovskites

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  18. Controlling the cation distribution and electric polarization with epitaxial strain in Aurivillius-phase Bi5FeTi3O15

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  19. Designing New Improper Ferroelectrics with a General Strategy

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  20. Two New Non-centrosymmetric n = 3 Layered Dion–Jacobson Perovskites: Polar RbBi2Ti2NbO10 and Nonpolar CsBi2Ti2TaO10

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  31. The role of Tb-doping on the structural and functional properties of Bi4−xTbxTi3O12 ferroelectric phases with the Aurivillius type structure

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  32. First-principles reinvestigation of bulk WO 3

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  33. Covalent and Ionic Functionalization of HLN Layered Perovskite by Sonochemical Methods

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  34. To superspace and beyond

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  35. Electronic, optical and thermoelectric properties of bulk and surface (001) CuInTe 2 : A first principles study

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  36. Designing new ferroelectrics with a general strategy

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  37. Ferroelectric properties of highly c -oriented epitaxial Bi 2 WO 6 thin films

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  38. Structural refinement of Pbnm-type perovskite films from analysis of half-order diffraction peaks

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  39. On the “alpha-phase” of Ca2−xSrxMnO4 and extending the chemistry of Sr7−yCayMn4O15 to y>1

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  40. Polar Oxides without Inversion Symmetry through Vacancy and Chemical Order

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  41. Composition dependence of the multifunctional properties of Nd-doped Bi4Ti3O12 ceramics

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  42. Learning from data to design functional materials without inversion symmetry

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  44. Phase Transition Behavior of the Layered Perovskite CsBi0.6La0.4Nb2O7: A Hybrid Improper Ferroelectric

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  45. Atomic Layer Engineering of High-κ Ferroelectricity in 2D Perovskites

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  46. Structural Modification of the Cation-Ordered Ruddlesden–Popper Phase YSr2Mn2O7 by Cation Exchange and Anion Insertion

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  47. Designing of metallic nanocrystals embedded in non-stoichiometric perovskite nanomaterial and its surface-electronic characteristics

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  48. Electric-Magneto-Optical Kerr Effect in a Hybrid Organic–Inorganic Perovskite

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  49. First-principles study of tungsten trioxide: Structural properties and polaron formation

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  50. Magnetic and ferroelectric properties of Aurivillius phase Bi7Fe3Ti3O21 and their doped films

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