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Register a new userManipulating Ferroelectric Domains in Nanostructures Under Electron Beams
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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.
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Ferroelectric random access memory cells (FeRAMs) have reached 450 x 400 nm production (0.18 micron^2) at Samsung with lead zirconate-titanate (PZT), 0.13 micron^2 at Matsushita with strontium bismuth tantalate (SBT), and comparable sizes at Fujitsu with BiFeO3. However, in order to increase storage density, the industry roadmap requires by 2010 that such planar devices be replaced with three-dimensional structures. Unfortunately, little is known yet about even such basic questions as the domain scaling of 3-d nanodevices, as opposed to 2-d thin films. Here we report the experimental measurement of nano-domains in ferroelectric nanocolumns, together with a theory of domain size in 3-d structures which explains the observations.
Ferroelectrics display spontaneous and switchable electrical polarization. Until recently, ferroelectricity was believed to disappear at the nanoscale; now, nano-ferroelectrics are being considered in numerous applications. This renewed interest was partly fuelled by the observation of ferroelectric domains in films of a few unit cells thickness, promising further size reduction of ferroelectric devices. It turns out that at reduced scales and dimensionalities the materials properties depend crucially on the intricacies of domain formation, that is, the way the crystal splits into regions with polarization oriented along the different energetically equivalent directions, typically at 180o and 90o from each other. Here we present a step forward in the manipulation and control of ferroelectric domains by the growth of thin films with regular self-patterned arrays of 90o domains only 7 nm wide. This is the narrowest width for 90o domains in epitaxial ferroelectrics that preserves the film lateral coherence, independently of the substrate.
Local-probe imaging of the ferroelectric domain structure and auxiliary bulk pyroelectric measurements were conducted at low temperatures with the aim to clarify the essential aspects of the orbitally driven phase transition in GaMo4S8, a lacunar spinel crystal that can be viewed as a spin-hole analogue of its GaV4S8 counterpart. We employed multiple scanning probe techniques combined with symmetry and mechanical compatibility analysis to uncover the hierarchical domain structures, developing on the 10-100 nm scale. The identified domain architecture involves a plethora of ferroelectric domain boundaries and junctions, including primary and secondary domain walls in both electrically neutral and charged configurations, and topological line defects transforming neutral secondary walls into two oppositely charged ones.
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.
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.
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