Tilt engineering of spontaneous polarization and magnetization above 300 K in a bulk layered perovskite

Pitcher, Michael J.; Mandal, P.; Dyer, Matthew S.; Alaria, Jonathan; Borisov, Pavel; Niu, Hongjun; Claridge, John B.; Rosseinsky, Matthew J.

doi:10.1126/science.1262118

Cited by 202 publications

(188 citation statements)

References 40 publications

(1 reference statement)

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“…Due to their unusual lattice couplings and dynamics, there has been renewed recent interest in tuning the properties of layered materials based on the perovskite structure, including proper, 1,2 and improper, [3][4][5] ferroelectricity, the electrocaloric effect, 6 and colossal magnetoresistance. 7 Unprecedented control of ferroelectricity in layered perovskites has been achieved, for example, by engineering non-polar lattice instabilities that can combine in the ground state to produce a net polarisation.…”

Section: Introductionmentioning

confidence: 99%

The origin of uniaxial negative thermal expansion in layered perovskites

et al. 2017

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Why is it that ABO 3 perovskites generally do not exhibit negative thermal expansion (NTE) over a wide temperature range, whereas layered perovskites of the same chemical family often do? It is generally accepted that there are two key ingredients that determine the extent of NTE: the presence of soft phonon modes that drive contraction (have negative Grüneisen parameters); and anisotropic elastic compliance that predisposes the material to the deformations required for NTE along a specific axis. This difference in thermal expansion properties is surprising since both ABO 3 and layered perovskites often possess these ingredients in equal measure in their high-symmetry phases. Using first principles calculations and symmetry analysis, we show that in layered perovskites there is a significant enhancement of elastic anisotropy due to symmetry breaking that results from the combined effect of layering and condensed rotations of oxygen octahedra. This feature, unique to layered perovskites of certain symmetry, is what allows uniaxial NTE to persist over a large temperature range. This fundamental insight means that symmetry and the elastic tensor can be used as descriptors in high-throughput screening and to direct materials design.

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Section: Introductionmentioning

confidence: 99%

The origin of uniaxial negative thermal expansion in layered perovskites

et al. 2017

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“…There has been a large amount of renewed interest in improper ferroelectric mechanisms recently, particularly in studying the coupling between two nonpolar zone-boundary lattice modes with octahedral tilt character in the RuddlesdenPopper layered perovskites, which has been discussed in the context of "hybrid improper ferroelectricity" [2,[35][36][37]. Here we reveal a mechanism by which two zone-boundary modes, implicitly dependent on orbital degrees of freedom, combine to give polar zone-centered displacements.…”

Section: Charge Ordering and Improper Ferroelectric Couplingmentioning

confidence: 99%

“…Unfortunately, the measurements of pyrocurrent or polarization-electric field (PE) loops in the P nn2 phase at higher temperatures above the magnetic ordering transition has been impossible due to leakage currents at these higher temperatures. Obtaining such direct measures of the switchable nature of the crystallographically identified polar ground state is a substantial future challenge for this and other recently reported hybrid improper ferroelectrics [2,35]. Our following discussion on ferroelectric switching pathways is based on symmetry arguments alone.…”

Section: Charge Ordering and Improper Ferroelectric Couplingmentioning

confidence: 99%

Improper ferroelectric polarization in a perovskite driven by intersite charge transfer and ordering

Chen

Wang

et al. 2018

Phys. Rev. B

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It is of great interest to design and make materials in which ferroelectric polarization is coupled to other order parameters such as lattice, magnetic, and electronic instabilities. Such materials will be invaluable in next-generation data storage devices. Recently, remarkable progress has been made in understanding improper ferroelectric coupling mechanisms that arise from lattice and magnetic instabilities. However, although theoretically predicted, a compact lattice coupling between electronic and ferroelectric (polar) instabilities has yet to be realized. Here we report detailed crystallographic studies of a perovskite Hg A MnO 12 that is found to exhibit a polar ground state on account of such couplings that arise from charge and orbital ordering on both the A -and B-sites, which are themselves driven by a highly unusual Mn A -Mn B intersite charge transfer. The inherent coupling of polar, charge, orbital, and hence magnetic degrees of freedom make this a system of great fundamental interest, and demonstrating ferroelectric switching in this and a host of recently reported hybrid improper ferroelectrics remains a substantial challenge.

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“…al. [24] on polar double perovskite (Ca y Sr 1−y ) 1.15 Tb 1.85 Fe 2 O 7 has shown that the polarization and magnetization in this material co-exist at room temperature and that the polarization is induced through a hybrid improper mechanism. Hence, it appears that HIF may be a promising and practical means to design new magnetoelectrics (MEs).…”

Section: Introductionmentioning

confidence: 99%

Linear magnetoelectricity at room temperature in perovskite superlattices by design

2015

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Discovering materials that display a linear magnetoelectric (ME) effect at room temperature is a challenge. Such materials could facilitate novel devices based on the electric-field control of magnetism. Here we present simple, chemically intuitive design rules to identify a new class of bulk magnetoelectric materials based on the 'bicolor' layering of P bnm ferrite perovskites, e.g., LaFeO3/ LnFeO3 superlattices, Ln = lanthanide cation. We use first-principles density-functional theory calculations to confirm these ideas. We elucidate the origin of this effect and show it is a general consequence of the layering of any bicolor, P bnm perovskite superlattice in which the number of constituent layers are odd (leading to a form of hybrid improper ferroelectricity). Our calculations suggest that the ME effect in these superlattices is larger than that observed in the prototypical magnetoelectric materials Cr2O3 and BiFeO3. Furthermore, in these proposed materials, the strength of the linear ME coupling increases with the magnitude of the induced spontaneous polarization which is controlled by the La/Ln cation radius mismatch. We use a simple mean field model to show that the proposed materials order magnetically above room temperature.

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Tilt engineering of spontaneous polarization and magnetization above 300 K in a bulk layered perovskite

Cited by 202 publications

References 40 publications

The origin of uniaxial negative thermal expansion in layered perovskites

The origin of uniaxial negative thermal expansion in layered perovskites

Improper ferroelectric polarization in a perovskite driven by intersite charge transfer and ordering

Linear magnetoelectricity at room temperature in perovskite superlattices by design

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