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Contact-free reversible switching of improper ferroelectric domains by electron and ion irradiation

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 Added by Dennis Meier
 Publication date 2020
  fields Physics
and research's language is English




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Focused ion beam (FIB) and scanning electron microscopy (SEM) are used to reversibly switch improper ferroelectric domains in the hexagonal manganite ErMnO$_3$. Surface charging is achieved by local ion (positive charging) and electron (positive and negative charging) irradiation, which allows controlled polarization switching without the need for electrical contacts. Polarization cycling reveals that the domain walls tend to return to the equilibrium configuration obtained in the as-grown state. The electric field response of sub-surface domains is studied by FIB cross-sectioning, revealing the 3D switching behavior. The results clarify how the polarization reversal in hexagonal manganites progresses at the level of domains, resolving both domain wall movements and the nucleation and growth of new domains. Our FIB-SEM based switching approach is applicable to all ferroelectrics where a sufficiently large electric field can be built up via surface charging, facilitating contact-free high-resolution studies of the domain and domain wall response to electric fields in 3D.



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Improper ferroelectrics are described by two order parameters: a primary one, driving a transition to long-range distortive, magnetic or otherwise non-electric order, and the electric polarization, which is induced by the primary order parameter as a secondary, complementary effect. Using low-temperature scanning probe microscopy, we show that improper ferroelectric domains in YMnO$_3$ can be locally switched by electric field poling. However, subsequent temperature changes restore the as-grown domain structure as determined by the primary lattice distortion. The backswitching is explained by uncompensated bound charges occuring at the newly written domain walls due to the lack of mobile screening charges at low temperature. Thus, the polarization of improper ferroelectrics is in many ways subject to the same electrostatics as in their proper counterparts, yet complemented by additional functionalities arising from the primary order parameter. Tailoring the complex interplay between primary order parameter, polarization, and electrostatics is therefore likely to result in novel functionalities specific to improper ferroelectrics.
Field-induced switching of ferroelectric domains with a topological vortex configuration is studied by atomic imaging and electrical biasing in an electron microscope, revealing the role of topological defects on the topologically-guided change of domain-wall pairs in a hexagonal manganite.
Freestanding BaTiO3 nanodots exhibit domain structures characterized by distinct quadrants of ferroelastic 90{deg} domains in transmission electron microscopy (TEM) observations. These differ significantly from flux-closure domain patterns in the same systems imaged by piezoresponse force microscopy. Based upon a series of phase field simulations of BaTiO3 nanodots, we suggest that the TEM patterns result from a radial electric field arising from electron beam charging of the nanodot. For sufficiently large charging, this converts flux-closure domain patterns to quadrant patterns with radial net polarizations. Not only does this explain the puzzling patterns that have been observed in TEM studies of ferroelectric nanodots, but also suggests how to manipulate ferroelectric domain patterns via electron beams.
The control of spin-dependent properties by voltage, not involving magnetization switching, has significant advantages for low-power spintronics. Here, we predict that the interfacial crystal Hall effect (ICHE) can serve for this purpose. We show that the ICHE can occur in heterostructures composed of compensated antiferromagnetic metals and non-magnetic insulators due to reduced symmetry at the interface, and it can be made reversible if the antiferromagnet is layered symmetrically between two identical ferroelectric layers. We explicitly demonstrate this phenomenon using density functional theory calculations for three material systems: MnBi$_{2}$Te$_{4}$/GeI$_{2}$ and topological In$_{2}$Te$_{3}$/MnBi$_{2}$Te$_{4}$/In$_{2}$Te$_{3}$ van der Waals heterostructures, and GeTe/Ru$_{2}$MnGe/GeTe heterostructure composed of three-dimensional materials. We show that all three systems reveal a sizable ICHE, while the latter two exhibit a quantum ICHE and ICHE, respectively, reversible with ferroelectric polarization. Our proposal opens an alternative direction for voltage controlled spintronics and offers not yet explored possibilities for functional devices by heterostructure design.
The origin of the unusual 90^o ferroelectric / ferroelastic domains, consistently observed in recent studies on meso and nanoscale free-standing single crystals of BaTiO3 [Schilling et al., Physical Review B, 74, 024115 (2006); Schilling et al., Nano Letters, 7, 3787 (2007)], has been considered. A model has been developed which postulates that the domains form as a response to elastic stress induced by a surface layer which does not undergo the paraelectric-ferroelectric, cubic-tetragonal phase transition. This model was found to accurately account for the changes in domain periodicity as a function of size that had been observed experimentally. The physical origin of the surface layer might readily be associated with patterning damage, seen in experiment; however, when all evidence of physical damage is removed from the BaTiO3 surfaces by thermal annealing, the domain configuration remains practically unchanged. This suggests a more intrinsic origin, such as the increased importance of surface tension at small dimensions. The effect of surface tension is also shown to be proportional to the difference in hardness between the surface and the interior of the ferroelectric. The present model for surface tension induced twinning should also be relevant for finely grained or core-shell structured ceramics.
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