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RESEARCH PAPER · Journal of the American Chemical Society · 2018

Hybrid 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 Phases

Suguru Yoshida, Hirofumi Akamatsu, Ryosuke Tsuji, Olivier Hernandez, Haricharan Padmanabhan, Arnab Sen Gupta, Alexandra S. Gibbs, Ko Mibu, Shunsuke Murai, James M. Rondinelli, Venkatraman Gopalan, Katsuhisa Tanaka, Koji Fujita

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Hybrid 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 PhasesOriginalNegative thermal expansion in high pressure layered perovskite Ca 2 GeO 410Electro‐Optic Modulation in Hybrid Metal Halide Perovskites64Hybrid improper ferroelectricity and possible ferroelectric switching paths in Sr3Hf2O720A -site cation size effect on oxygen octahedral rotations in acentric Ruddlesden-Popper alkali rare-earth titanates11Competing Polar and Antipolar Structures in the Ruddlesden–Popper Layered Perovskite Li2SrNb2O740First-order phase transition and unexpected rigid rotation mode in hybrid improper ferroelectric (La, Al) co-substituted Ca3Ti2O7 ceramics35High-temperature ferroelectric order and magnetoelectric coupling driven by the magnetic field cooling effect in R2BaCuO5(R=Er,Dy,Sm)16Weak Ferroelectricity in n = 2 Pseudo Ruddlesden–Popper-Type Niobate Li2SrNb2O736Temperature-Induced Structural Transformations in Undoped and Eu3+-Doped Ruddlesden–Popper Phases Sr2SnO4 and Sr3Sn2O7: Relation to the Impedance and Luminescence Behaviors13Tolerance Factor Control of Uniaxial Negative Thermal Expansion in a Layered Perovskite28Cadmium-based ferroelectrics with the Ruddlesden–Popper and double perovskite structures: a theoretical study9Ruddlesden–Popper perovskites in electrocatalysis330Phase Transition from Weak Ferroelectricity to Incipient Ferroelectricity in Li 2 Sr(Nb 1– x Ta x ) 2 O 728Enhanced hybrid improper ferroelectricity in Sr3−xBaxSn2O7 ceramics with a Ruddlesden–Popper (R–P) structure31Complex Structural Phase Transitions of the Hybrid Improper Polar Dion–Jacobson Oxides RbNdM 2 O 7 and CsNdM 2 O 7 (M = Nb, Ta)35Bi2W2O9 : A potentially antiferroelectric Aurivillius phase14Room-temperature ferroelectricity in A-site ordered Ruddlesden-Popper Li2CaTa2O7 ceramics21Improved hybrid improper ferroelectricity in B-site substituted Ca3Ti2O7 ceramics with a Ruddlesden–Popper structure21Ferroelectricity of Dion–Jacobson layered perovskites CsNdNb 2 O 7 and RbNdNb 2 O 720Exploring the A2BX3 Family for New Functional Materials Using Crystallographic Database Mining and First-Principles Calculations5Highly Tunable Ferroelectricity in Hybrid Improper Ferroelectric Sr3Sn2O740Polar Structures of KNdNb2O7and KNdTa2O710Discovery Principles and Materials for Symmetry-Protected Persistent Spin Textures with Long Spin Lifetimes33Tuning between Proper and Hybrid-Improper Mechanisms for Polar Behavior in Cs Ln 2Ti2NbO10 Dion-Jacobson Phases22Ca2MnO4 structural path: Following the negative thermal expansion at the local scale17Suppressing the ferroelectric switching barrier in hybrid improper ferroelectrics35Hybrid improper antiferroelectricity—New insights for novel device concepts2First-principle investigation of hybrid improper ferroelectricity of n = 2 Ruddlesden-Popper Sr3B2Se7 (B = Zr, Hf)0The influence of the 6s 2 configuration of Bi 3+ on the structures of A′BiNb 2 O 7 (A′ = Rb, Na, Li) layered perovskite oxides10Structural evolution and phase transition of Sr3Sn2O7 doped with Ca6Improved ferroelectric properties in hybrid improper ferroelectric Sr3−Ba Zr2O712Hybrid improper ferroelectricity in A-site cation ordered Li2La2Ti3O10 ceramic with triple-layer Ruddlesden–Popper structure13Coexisting Mechanisms for the Ferroelectric Phase Transition in Li2SrNb2O721Enhanced hybrid improper ferroelectricity in Fe/Nb cosubstituted Ca 3 Mn 2 O 7 ceramics16Group Theory Analysis to Study Phase Transitions of Quasi-2D Sr3Hf2O79Switching between Proper and Hybrid-Improper Polar Structures via Cation Substitution in A2La(TaTi)O7(A = Li, Na)17Expanding the Toolbox of Inorganic Mechanoluminescence Materials166Revealing pressure-driven structural transitions in the hybrid improper ferroelectric Sr 3 Sn 2 O 714Directed synthesis of a hybrid improper magnetoelectric multiferroic material25Free-Carrier-Induced Ferroelectricity in Layered Perovskites29Local-electrostatics-induced oxygen octahedral distortion in perovskite oxides and insight into the structure of Ruddlesden–Popper phases57Cocrystalline Polymer Films Exhibiting Second-Order Nonlinear Optical Properties7Octahedral rotations in Ruddlesden-Popper layered oxides under pressure from first principles11Review of experimental progress of hybrid improper ferroelectricity in layered perovskite oxides36Hybrid improper dipolar density wave in NaLaCoWO$_6$0The crystal and defect structures of polar KBiNb 2 O 72Designing new polar materials1Two-dimensional ferroelectricity induced by octahedral rotation distortion in perovskite oxides31Polarization-Enhanced Photovoltaic Effects in a High-Temperature Molecular Ferroelectric [C6N2H18][SbI5]-Based Solar Device19Hybrid improper dipolar density wave in NaLaCoWO61Disentangling types of lattice disorder impacting superconductivity in Sr2RuO4 by quantitative local probes12Phase variation of ferroelectric Li2Sr1−xCax(Nb1−xTax)2O7 by selective reinforcement in the (Nb,Ta)-O covalent bonds10Distortion modes and ferroelectric properties in hybrid improper ferroelectric Sr3(Sn,Zr)2O7 ceramics7Lone-Pair-Induced Intra- and Interlayer Polarizations in Sillén-Aurivillius Layered Perovskite Bi4NbO8Br23Hybrid Improper Ferroelectricity: A Theoretical, Computational, and Synthetic Perspective45Interplay between Oxygen Octahedral Rotation and Deformation in the Acentric ARTiO4 Series toward Negative Thermal Expansion19Suppression of Pressure-Induced Phase Transitions in a Monoclinically Distorted LiNbO3-Type CuNbO3 by Preference for a CuO3 Triangular Coordination Environment2Two-Dimensional Multiferroics with Intrinsic Magnetoelectric Coupling in A-Site Ordered Perovskite Monolayers25Controlling dielectric properties of Nb + X (X = Al, Ga, In) co-doped and Nb-doped rutile-type TiO 2 single crystals10Na 2 Ba[Na 2 Sn 2 S 7 ]: Structural Tolerance Factor‐Guided NLO Performance Improvement50Na2Ba[Na2Sn2S7]: Structural Tolerance Factor‐Guided NLO Performance Improvement0Ferroelectricity in oxygen-deficient perovskite-type oxide Sr 10 Ga 6 Sc 4 O 254Growth and Phase Transition of Sr3zr2o7 Single Crystals4Second Harmonic Generation in the Polar A′SmNb2O7 (A′ = Rb, Cs) Dion–Jacobson Layered Perovskites11Chemical Trends of Surface Reconstruction and Band Positions of Nonmetallic Perovskite Oxides from First Principles19Hybrid improper ferroelectricity and phase transition behavior of Li2Nd2Ti3O10 ceramics with A-site ordered triple-layer Ruddlesden-Popper structure6Scaling behavior of order parameters for the hybrid improper ferroelectric (Ca,Sr)3Ti2O75Influence of B‐site cation in lattice dynamics of bilayered Ruddlesden–Popper Sr3B2O7 (B = Zr, Mo, Sn, Hf) compounds11Confirmation of ferroelectricity, piezoelectricity, and crystal structure of the electronic dielectric TmFe2O410MnCaTa2O7─A Magnetically Ordered Polar Phase Prepared via Cation Exchange4The novel electrical properties in quasi‐2D hybrid improper ferroelectric Sr 3 Sn 2 O 7 ceramic and the structural modulation6Competing polar and antipolar phases in n=2 Ruddlesden-Popper niobates and tantalates from first principles6Thermal multiferroics in all-inorganic quasi-two-dimensional halide perovskites21Polymorphism in the Ruddlesden–Popper Nickelate La 3 Ni 2 O 7 : Discovery of a Hidden Phase with Distinctive Layer Stacking123La 2 SrSc 2 O 7 : A -Site Cation Disorder Induces Ferroelectricity in Ruddlesden–Popper Layered Perovskite Oxide29Probing Ca 3 Ti 2 O 7 crystal structure at the atomic level: Insights from perturbed angular correlation spectroscopy and ab initio studies4Hybrid improper ferroelectricity in La2Sr (Sc1− x Fe x )2O7 ceramics with double-layered Ruddlesden–Popper structures10Simultaneous manipulation of ferroic order in multiferroic materials2Piezoelectricity in n = 2 Ruddlesden–Popper Ferroelectric Oxides9Ferroelectricity Induced by a Combination of Crystallographic Chirality and Axial Vector7Effects of doping with magnetic cations on the hybrid improper ferroelectricity in Sr3Sn2O73Tolerance Factor Approach for the Design of Quaternary Materials as Applied to the A2Ln4Cu2nQ7+n Homologous Series7Experimental Evidence of Piezoelectricity and Ferroelectricity in Electronic Dielectrics TmFe2O40Imaging Ferroelastic Domain Walls in Hybrid Improper Ferroelectric Sr3Sn2O713Theoretical and data-driven approaches to semiconductors and dielectrics: from prediction to experiment2Structural frustration effects by mixed alkali ions in ferroelectric Dion–Jacobson layered perovskites (Cs,Rb)NdNb 2 O 76Suppression of Ferroelectric Transitions by Symmetry Trapping in Dion–Jacobson-Layered Perovskites Cs(La,Nd)Nb2O74Perspective on 2D perovskite ferroelectrics and multiferroics12Interplay between A-site and oxygen-vacancy ordering, and mixed electron/oxide-ion conductivity in n = 1 Ruddlesden–Popper perovskite Sr 2 Nd 2 Zn 2 O 77Hybrid improper ferroelectricity in a Si-compatible CeO2/HfO2 artificial superlattice2Recent Progress of Hybrid Improper Ferroelectrics with Ruddlesden-Popper Structure1Thermally Controlled A-site Cation Ordering and Coupled Polarity in Double Perovskite NaLaZr2O62Interplay between Jahn–Teller Distortions and Structural Phase Transitions in Ruddlesden–Poppers21Exploring the magnetic percolation threshold in the improper ferroelectric Sr3Sn2O7 upon Cr and Fe-doping4Dion–Jacobson (n = 2) Layered Perovskites (A′SmTa2O7; A′ = Rb, Cs) As Potential Ferroelectric Materials6The varying temperature- and pressure-induced phase transition pathways in hybrid improper ferroelectric Sr 3 Sn 2 O 72Giant Shear-vertical Wave Bandgaps Induced by Diffuse Domain-walls in Ferroelectrics6Significantly enhanced stability of hybrid improper ferroelectricity in Sr 3 Zr 2 O 7 by isovalent Ca substitution1Competing Octahedral Modes in the Hybrid Improper Ruddlesden–Popper Ferroelectric Ln 2 SrSc 2 O 78Cation Exchange as a Route to Introduce Magnetism to Hybrid-Improper Polar Phases0Temperature-induced structural phase transitions in inorganic compounds: symmetry and information-entropy analysis1A-Site Cation Disorder Engineering in Ruddlesden–Popper Layered Perovskite Oxide La 2 (Ba,Sr)In 2 O 7 for Hybrid Improper Ferroelectricity8Perovskite nanostructures as effective bifunctional acid-base heterogenous catalysts for biodiesel production: A comprehensive review7Exploring a route to induce ferromagnetism on Sr3Sn2O7 by co-doping with non-Jahn-Teller-distorted Mn3+ and La3+ cations1Theoretical investigation of noncentrosymmetric Ruddlesden-Popper germanium perovskites Cs 2 Ge X 4 ( X = Cl , Br, and I) for second harmonic generation0Hybrid improper ferroelectricity and phase transition in La2Sr(Sc1− x In x )2O7 ceramics2A study focusing on the influence of multiple cationic substitutions in Dion–Jacobson ( n = 2) layered perovskite oxides0a-axis stacking of Quasi-2D Ruddlesden–Popper (RP) Sr3Sn2O7 ceramics show strong in-plane piezoresponse0Crystal structures, dielectric properties, and phase transition in hybrid improper ferroelectric Li2Sm2Ti3O10 ceramics0Crystal structures, dielectric properties, and thermal behavior in hybrid improper ferroelectric Li2Sm2Ti3O10 ceramics0Revival of Layered Ferroelectrics in Thin Films2Tunable polarization and band gap in ferroelectric nitride perovskites via superlattice design0Controlling the competition between polar and antipolar structures by rumpling in Ruddlesden–Popper layered nitride La3W2N70Kinetic control of A-site cation disorder and its impact on the ferroelectric phase transition in La2SrSc2O7 layered perovskite oxide3Defect‐Engineered IrO x @Perovskite Heterostructures via Thermal Reconstruction for Acid‐Stable Oxygen Evolution Catalysis1Multiferroic phase transition between multiple types of collinear compensated magnets3Redox-Neutral Interstitial Hydride Incorporation in Ruddlesden–Popper Oxides0The role of space group symmetry in BiFeO3 for multifunctional energy harvesting applications0Structure–Property Relations in Metal-Substituted Polar Chalcogenides under Pressure1Record‐Low Coercive Field and Stable Curie Temperature in Bulk Hybrid Improper Ferroelectrics via Synergistic A / B ‐Site Co‐Substitution0Cation Coordination Preferences toward Stacking Design in Layered Perovskites along the Perovskite [111] Direction0Hybrid improper ferroelectricity and enhanced Curie temperature in co-substituted La2SrSc2O7-based ceramics0

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  45. Hybrid improper dipolar density wave in NaLaCoWO$_6$

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  47. Designing new polar materials

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  48. Two-dimensional ferroelectricity induced by octahedral rotation distortion in perovskite oxides

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  49. Polarization-Enhanced Photovoltaic Effects in a High-Temperature Molecular Ferroelectric [C6N2H18][SbI5]-Based Solar Device

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  50. Hybrid improper dipolar density wave in NaLaCoWO6

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    Andrea Griesi, Enrico Mugnaioli, Arianna Lanza, Valentina Vit, L. Righi, Mauro Gemmi, Fabio Orlandi

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