<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mrow><mml:mtext>SrTiO</mml:mtext></mml:mrow><mml:mn>3</mml:mn></mml:msub></mml:mrow></mml:math>and<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mrow><mml:mtext>BaTiO</mml:mtext></mml:mrow><mml:mn>3</mml:mn></mml:msub></mml:mrow></mml:math>revisited using the projector augmented wave method: Performance of hybrid and semilocal functionals

Wahl, Roman; Vogtenhuber, Doris; Kresse, Georg

doi:10.1103/physrevb.78.104116

Cited by 235 publications

(226 citation statements)

References 58 publications

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“…We find for unstrained BaTiO 3 a 0 =3.93Å and c/a = 1.007, which are close to the values in other calculations (for instance, a 0 = 3.945Å and c/a = 1.009 in Ref. 39).…”

Section: Structural Optimizationsupporting

confidence: 77%

Mode sequence, frequency change of nonsoft phonons, and LO-TO splitting in strained tetragonalBaTiO3

Raeliarijaona

2015

Phys. Rev. B

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Ultraviolet Raman spectroscopy revealed the existence of an unusual large frequency shift occurring to a non-soft mode of E(TO4) when BaTiO3 is strained to a SrTiO3 substrate [D. Tenne et al., Science 313, 1614]. It raised two interesting questions: (i) whether there are other non-soft modes that possess similar or even larger strain-induced frequency shifts; (ii) how the mode sequence is altered by these shifts in frequency. Note that mode sequence is also pivotal in correctly indexing and assigning the spectroscopy peaks observed in all Raman experiments. By mapping out the evolutions of individual phonon modes as a function of strain using first-principles density functional perturbation calculations, we determine the mode sequence and strain-induced phonon frequency shifts in prototypical BaTiO3. Our study reveals that the mode sequence is drastically different when BaTiO3 is strained to SrTiO3 as compared to that in the unstrained structure, caused by multiple mode crossings. Furthermore, we predict that three other non-soft modes-A1(TO2), E(LO4), and A1(TO3)-display even larger strain-induced frequency shifts than E(TO4). The strain responses of individual modes are found to be highly mode specific, and a mechanism that regulates the magnitude of the frequency shift is provided. As another key outcome of this study, we tackle a long-standing problem of LO-TO splitting in ferroelectrics. A rigorous definition for the LO-TO splitting is formulated, which allows this critical quantity to be calculated quantitatively. The definition immediately reveals a new finding, that is, a large LO-TO splitting not only exists for E(LO4), which is previously known and originates from a soft mode, it also occurs to a non-soft A1(LO3) mode. The LO-TO splitting is shown to decrease drastically with compressive strain, and this decrease cannot be explained by the Born effective charges and high-frequency dielectric constants.

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“…We find for unstrained BaTiO 3 a 0 =3.93Å and c/a = 1.007, which are close to the values in other calculations (for instance, a 0 = 3.945Å and c/a = 1.009 in Ref. 39).…”

Section: Structural Optimizationsupporting

confidence: 77%

Mode sequence, frequency change of nonsoft phonons, and LO-TO splitting in strained tetragonalBaTiO3

Raeliarijaona

2015

Phys. Rev. B

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“…Out of twelve optical modes, three triply-degenerate phonon modes have Γ 15 symmetry and one triply-degenerate mode has Γ 25 symmetry. The eigenvector of the phonon mode with Γ 25 symmetry involves atomic displacements along the z direction are better than earlier theoretically-calculated values using different functionals 14,42,43 .…”

Section: Vibrational Propertiesmentioning

confidence: 61%

Accuracy of first-principles interatomic interactions and predictions of ferroelectric phase transitions in perovskite oxides: Energy functional and effective Hamiltonian

et al. 2017

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While first-principles density functional theory (DFT) based models have been effective in capturing the physics of ferroelectric phase transitions in BaTiO 3 , PbTiO 3 and KNbO 3 , quantitative estimates of the transition temperatures (T C 's) suffer from errors that are believed to originate from the errors in estimating lattice constants obtained within local density (LDA) and gradient density (GGA) approximations of DFT. The recently-developed strongly constrained and appropriately normed (SCAN) meta-GGA functional has been shown to be quite accurate in estimation of lattice constants. Here, we present a quantitative analysis of the estimates of ferroelectric ground state properties of eight perovskite oxides and transition temperatures of BaTiO 3 , PbTiO 3 and KNbO 3 obtained with molecular dynamics (MD) simulations using an effective Hamiltonian derived from the SCAN meta-GGA based DFT. Relative to LDA, we find an improvement in estimates of T C 's, which arises from the changes in calculated strain-phonon, anharmonic coupling constants and strength of ferroelectric instabilities, i.e., frequencies of the soft modes. We also assess the errors in T C originating from approximately integrating out the high-energy phonons during construction of the model Hamiltonian through estimates of the effects of fourth-order couplings between soft mode and higher energy modes of BaTiO 3 , PbTiO 3 and KNbO 3 . We find that inclusion of these anharmonic couplings results in deeper double-well energy functions of ferroelectric distortions and further improvement in the estimates of transition temperatures. Consistently improved estimates of lattice constants and transition temperatures with the SCAN meta-GGA calculations augur well for their use in simulations of superlattices or hetero-structures of perovskite oxides, in which the effects of lattice matching are critical.

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“…This materials design framework for achieving large electrical polarizations and low switching barriers will be a crucial guide to the successful integration of these new multifunctional ferroelectric materials into next generation devices. 34 , which provides an improved description of structure 34 over LDA or PBE 35 . We used a plane wave energy cutoff of 650 eV.…”

Section: Discussionmentioning

confidence: 99%

Turning ABO₃ Antiferroelectrics into Ferroelectrics: Design Rules for Practical Rotation‐Driven Ferroelectricity in Double Perovskites and A₃B₂O₇ Ruddlesden‐Popper Compounds

Mulder

Benedek

Rondinelli

et al. 2013

Adv Funct Materials

287

291

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I. ABSTRACTFerroic transition metal oxides, which exhibit spontaneous elastic, electrical, magnetic or toroidal order, exhibit functional properties that find use in ultrastable solid-state memories to sensors and medical imaging technologies. To realize multifunctional behavior, where one order parameter can be coupled to the conjugate field of another order parameter, however, requires a common microscopic origin for the long-range order. Here, we formulate a complete theory for a novel form of ferroelectricity, whereby a spontaneous and switchable polarization emerges from the destruction of an antiferroelectric state due to octahedral rotations and ordered cation sublattices. We then construct a materials design framework based on crystal-chemistry descriptors rooted in group theory, which enables the facile design of artificial oxides with large electric polarizations, P , simultaneous with small energetic switching barriers between +P and -P . We validate the theory with first principles density functional calculations on more than 16 perovskite-structured oxides, illustrating it could be operative in any materials classes exhibiting two-or three-dimensional cornerconnected octahedral frameworks. We show the principles governing materials selection of the "layered" systems originate in the lattice dynamics of the A cation displacements stabilized by the pervasive BO 6 rotations of single phase ABO 3 materials, whereby the latter distortions govern the optical band gaps, magnetic order and critical transition temperatures. Our approach provides the elusive route to the ultimate multifunctionality property control by an external electric field. II. INTRODUCTIONIn the search for new classes of multifunctional materials, the design or discovery of ferroelectrics in which the spontaneous electrical polarization couples strongly to other structural, magnetic, orbital, and electronic degrees of freedom is a challenge being actively pursued as a means to achieve electric field-controllable emergent phenomena such as ferromagnetism 1,2 . Much of the current materials-by-design effort has focused on the structurally and chemically complex ABO 3 perovskites, a large class of functional materials that display a wide range of properties due to their highly tunable ground states. Because of the high susceptibility of perovskite materials towards polar structural instabilities, a notion has emerged that it is generally more productive to start with a material that displays, for example, ferromagnetism, and devise a way to induce ferroelectricity. Two highly successful approaches that have captivated the attention of researchers over the last decade are that of epitaxial strain engineering (strain-induced ferroelectricity, mutliferroicity) and that of selective chemical substitution of a stereochemically inactive cation with a lone-pair-active cation such as Bi 3+ , as in BiFeO 3 3,4 . While highly successful at creating new multiferroics (materials that are both ferromagnetic and ferroelectric), generally speaking these ...

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SrTiO3andBaTiO3revisited using the projector augmented wave method: Performance of hybrid and semilocal functionals

Cited by 235 publications

References 58 publications

Mode sequence, frequency change of nonsoft phonons, and LO-TO splitting in strained tetragonalBaTiO3

Mode sequence, frequency change of nonsoft phonons, and LO-TO splitting in strained tetragonalBaTiO3

Accuracy of first-principles interatomic interactions and predictions of ferroelectric phase transitions in perovskite oxides: Energy functional and effective Hamiltonian

Turning ABO₃ Antiferroelectrics into Ferroelectrics: Design Rules for Practical Rotation‐Driven Ferroelectricity in Double Perovskites and A₃B₂O₇ Ruddlesden‐Popper Compounds

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SrTiO3andBaTiO3revisited using the projector augmented wave method: Performance of hybrid and semilocal functionals

Cited by 235 publications

References 58 publications

Mode sequence, frequency change of nonsoft phonons, and LO-TO splitting in strained tetragonalBaTiO3

Mode sequence, frequency change of nonsoft phonons, and LO-TO splitting in strained tetragonalBaTiO3

Accuracy of first-principles interatomic interactions and predictions of ferroelectric phase transitions in perovskite oxides: Energy functional and effective Hamiltonian

Turning ABO3 Antiferroelectrics into Ferroelectrics: Design Rules for Practical Rotation‐Driven Ferroelectricity in Double Perovskites and A3B2O7 Ruddlesden‐Popper Compounds

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Turning ABO₃ Antiferroelectrics into Ferroelectrics: Design Rules for Practical Rotation‐Driven Ferroelectricity in Double Perovskites and A₃B₂O₇ Ruddlesden‐Popper Compounds