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Effect of the Degree of Overcooling on Relaxation of the Domain Structure of Triglycine Sulphate

The formation and evolution of the domain structure in the vicinity of the Curie point is studied in triglycine sulfate crystals subjected to fast cooling T{sub C}. We derive an analytical expression for time dependence of the mean characteristic domain size. This expression enable us to investigate the process of enlargement of domain structure through all stages of its relaxation into a state of thermodynamic equilibrium. The model predicts a root-square behavior of the mean domain size, which agrees well with available experimental data. The rate of enlargement of the domain structure is shown to depend on the degree of overcooling. The time dependence of the mean domain size obtained in this study enables us to determine the radius of intermolecular interactions in the crystals under study.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

The influence of cooling rates on strain phase diagrams and domain structures of ferroelectric thin films: A case study of PbTiO 3

Strain engineering has been established as an effective approach to control phase equilibria, domain configurations, and functional properties of ferroelectric thin films. Temperature-strain phase diagrams have been used as powerful tools for providing insights into strain engineering. However, almost all existing phase diagrams established using the phase-field approach assume quenching conditions without considering actual cooling rates during the post-deposition annealing process of ferroelectric thin films. Within this work, we systematically investigate the influence of cooling rates on domain structures and the strain-phase diagram of ferroelectric thin films using phase-field simulations, taking PbTiO 3 thin films as a model system. We found that both the position of phase boundaries in the strain phase diagrams and the domain morphology are significantly influenced by the cooling rates. It is revealed that while the paraelectric-ferroelectric phase boundary remains invariant, the phase boundaries between single-phase and multi-phase regions tend to shift toward the corresponding multi-phase region as the cool rate reduces. Slow cooling generally leads to more ordered domain structures with increased domain size. Using the obtained equilibrium domain structures, we calculated effective thermal conductivities and found significant variations that can be tuned by the cooling rates. In conclusion, this work reveals an underexplored yet critical impact of cooling rates on phase equilibria and domain structures in ferroelectric thin films, which may inspire further fine-tuning of domains and domain walls in low-dimensional ferroelectrics for multifunctional applications.

Domain structures↗

Phase transitions, domain structure, and pseudosymmetry in La- and Ti-doped BiFeO{sub 3}

The phase transitions and domain structure of the promising PbO-free solid solution series, (0.95-x)BiFeO{sub 3}-xLaFeO{sub 3}-0.05La{sub 2/3}TiO{sub 3}, were investigated. X ray diffraction (XRD) revealed a transition from a ferroelectric R3c to a PbZrO{sub 3}-like (Pbam) antiferroelectric (AFE) structure at x = 0.15 followed by a transition to a paraelectric (PE, Pnma) phase at x > 0.30. The ferroelastic/ferroelectric twin domain width decreased to 10–20 nm with increasing x as the AFE phase boundary was approached but coherent antiphase tilted domains were an order of magnitude greater. This domain structure suggested the local symmetry (20 nm) is lower than the average structure (R3c, a{sup −}a{sup −}a{sup −}) of the tilted regions. The PE phase (x = 0.35) exhibited a dominant a{sup −}a{sup −}c{sup +} tilt system with Pnma symmetry but diffuse reflections at ∼1/4(ooe) positions suggest that short range antipolar order is residual in the PE phase. The complex domain structure and phase assemblage of this system challenge the conventional interpretation of phase transitions based on macroscopic symmetry. Instead, it supports the notion that frustration driven by chemical distributions at the nanometric level influences the local or pseudo-symmetry as well as the domain structure, with XRD giving only the average macroscopic structure.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Toward Decoding the Relationship between Domain Structure and Functionality in Ferroelectrics via Hidden Latent Variables

Polarization switching mechanisms in ferroelectric materials are fundamentally linked to local domain structure and the presence of the structural defects, which both can act as nucleation and pinning centers and create local electrostatic and mechanical depolarization fields affecting wall dynamics. However, the general correlative mechanisms between domain structure and polarization dynamics are only weakly explored, precluding insight into the associated physical mechanisms. In this work, the correlation between local domain structures and switching behavior in ferroelectric materials is explored using convolutional encoder–decoder networks, enabling image to spectral (im2spec) and spectral to image (spec2im) translations via encoding of latent variables. The latter reflect the assumption that the relationship between domain structure and polarization switching is parsimonious, i.e., is based upon a small number of local mechanisms. The analysis of latent variables distributions and their real-space representations provides insight into the predictability of the local switching behavior and hence associated physical mechanisms. We further pose that the regions where these correlative relationships are violated, i.e., predictability of the polarization dynamics from domain structure is reduced, represent the obvious target for detailed studies, e.g., in the context of automated experiments. This approach provides a workflow to establish the presence of correlation between local spectral responses and local structure and can be universally applied to spectral imaging techniques such as piezoresponse force microscopy (PFM), scanning tunneling microscopy (STM) and spectroscopy, and electron energy loss spectroscopy (EELS) in scanning transmission electron microscopy (STEM).

36 MATERIALS SCIENCE↗

An in-situ study of magnetic domain structures in undercooled Fe-29.5 at. %Pd magnetostrictive alloys by Lorentz microscopy and electron holography

Understanding of correlation between magnetic domain structure and functional properties is of importance for the magnetic field driven phase transition (e.g., martensitic transformation) or microstructure variation (e.g., twin boundary motion) materials. In this work, we report a Fe-29.5 at. %Pd shape memory alloy treated by undercooling processing upon a degree of 320 K below the liquid temperature. The effect of high undercooling on the solidified microstructure and martensitic transformation temperatures was investigated. By in-situ Lorentz transmission electron microscopy and electron holography, magnetic domain structure and the field-induced domain wall motion behavior in as-cast and undercooled samples have been schematically studied. The irregular domain structure can be observed in these alloys. On the application of a field up to 300 Oe, the domain walls for both samples are able to move along the direction of the external magnetic field, but structural transition and rearrangement of variants are not observed in the undercooled alloy. The large magnetostriction of Fe-29.5 at. %Pd undercooled alloy originates from the irregular domain walls motion instead of the rearrangement of martensitic twin variants.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Specific Features of the Domain Structure of BaTiO{sub 3} Crystals during Thermal Heating and Cooling

This paper presents the results of the study of the domain structure of barium titanate crystals in a wide temperature range including the Curie point (T{sub C}) using the polarization-optical method in the reflected light and the force microscopy of the piezoelectric response. It is shown that a new a–c domain structure forms during cyclic heating of the crystal above T{sub C} and subsequent cooling to the ferroelectric phase. The role of uncompensated charges appeared on the crystal surface during the phase transition and their influence on the formation of the domain structure during cooling are discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Simulations of super-structure domain walls in two dimensional assemblies of magnetic nanoparticles

We simulate the formation of domain walls in two-dimensional assemblies of magnetic nanoparticles. Particle parameters are chosen to match recent electron holography and Lorentz microscopy studies of almost monodisperse cobalt nanoparticles assembled into regular, elongated lattices. As the particles are small enough to consist of a single magnetic domain each, their magnetic interactions can be described by a spin model in which each particle is assigned a macroscopic “superspin.” Thus, the magnetic behaviour of these lattices may be compared to magnetic crystals with nanoparticle superspins taking the role of the atomic spins. The coupling is, however, different. The superspins interact only by dipolar interactions as exchange coupling between individual nanoparticles may be neglected due to interparticle spacing. We observe that it is energetically favorable to introduce domain walls oriented along the long dimension of nanoparticle assemblies rather than along the short dimension. This is unlike what is typically observed in continuous magnetic materials, where the exchange interaction introduces an energetic cost proportional to the area of the domain walls. Structural disorder, which will always be present in realistic assemblies, pins longitudinal domain walls when the external field is reversed, and makes a gradual reversal of the magnetization by migration of longitudinal domain walls possible, in agreement with previous experimental results.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Domain structures and magnetization reversal in Co/Pd and CoFeB/Pd multilayers

Domain structures and magnetization reversal of (Co/Pd) and (CoFeB/Pd) multilayers with 7 and 14 repeats were investigated. The Co-based multilayers show much larger coercivities, a better squareness, and a sharper magnetization switching than CoFeB-based multilayers. From magnetic force microscopy observations, both structures show strong reduction in domains size as the number of repeats increases but the magnetic domains for Co-based multilayers are more than one order of magnitude larger than for CoFeB-based multilayers. By imaging domains at different times, breaks in the (CoFeB/Pd) multilayer stripes were observed within only few hours, while no change could be seen for (Co/Pd) multilayers. Although CoFeB single layers are suitable for magnetoresistive devices due to their large spin polarization and low damping constants, their lamination with Pd suffers mainly from thermal instability.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Mapping of ferroelectric domain structure using angle-resolved piezoresponse force microscopy

Angle-resolved piezoresponse force microscopy (AR-PFM) was used in conjunction with electron backscatter diffraction (EBSD) to study ferroelectric domain structure in polycrystalline near-morphotropic lead zirconate titanate (PZT). We introduce the details of AR-PFM including experimental method, the process to generate AR-PFM maps, and the interpretation of AR-PFM map, using domain patterns observed in bulk PZT. The spatial distortion caused by scanner creep and non-linearity in scanning probe microscopy was corrected through image registration, taking advantage of the features present in topography images. Domain structures were mapped using AR-PFM data, and the maps consistently show alternating piezoresponse axes in a lamellar pattern of non-180° domain structure. Comparison of AR-PFM and EBSD data showed a discrepancy between the direction of lateral surface displacement and the in-plane polarization direction. Additionally, using suitable domain patterns, AR-PFM enabled discrimination between the tetragonal and rhombohedral phases at the sub-grain scale.

36 MATERIALS SCIENCE↗

Controlling the anisotropy and domain structure with oblique deposition and substrate rotation

Effect of substrate rotation on anisotropy and domain structure for a thin ferromagnetic film has been investigated in this work. For this purpose Co films with 10 nm thickness have been prepared by sputtering with oblique angle of incidence for various substrate rotations. This method of preparation induces a uniaxial anisotropy due to shadow deposition effect. The magnetization reversal is studied by magneto-optic Kerr effect (MOKE) based microscope in the longitudinal geometry. The Co films prepared by rotating the substrate with 10 and 20 rpm weakens the anisotropy but does not completely give isotropic films. But this leads to high dispersion in local grain anisotropy resulting in ripple and labyrinth domains. It is observed that the substrate rotation has moderate effect on uniaxial anisotropy but has significant effect on the magnetization reversal process and the domain structure.

36 MATERIALS SCIENCE↗

Direct observation of temperature dependent magnetic domain structure of the multiferroic La{sub 0.66}Sr{sub 0.34}MnO{sub 3}/BiFeO{sub 3} bilayer system by x-ray linear dichroism- and x-ray magnetic circular dichroism-photoemission electron microscopy

Low-thickness La{sub 0.66}Sr{sub 0.34}MnO{sub 3} (LSMO)/BiFeO{sub 3} (BFO) thin film samples deposited on SrTiO{sub 3} were imaged by high resolution x-ray microscopy at different temperatures. The ultra-thin thickness of the top layer allows to image both the ferromagnetic domain structure of LSMO and the multiferroic domain structure of the buried BFO layer, opening a path to a direct observation of coupling at the interface on a microscopic level. By comparing the domain size and structure of the BFO and LSMO, we observed that, in contrast to LSMO single layers, LSMO/BFO multilayers show a strong temperature dependence of the ferromagnetic domain structure of the LSMO. Particularly, at 40 K, a similar domain size for BFO and LSMO is observed. This indicates a persistence of exchange coupling on the microscopic scale at a temperature, where the exchange bias as determined by magnetometer measurements is vanishing.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Mapping domain structures near a grain boundary in a lead zirconate titanate ferroelectric film using X-ray nanodiffraction

The effect of an electric field on local domain structure near a 24° tilt grain boundary in a 200 nm-thick Pb(Zr 0.2 Ti 0.8 )O 3 bi-crystal ferroelectric film was probed using synchrotron nanodiffraction. The bi-crystal film was grown epitaxially on SrRuO 3 -coated (001) SrTiO 3 24° tilt bi-crystal substrates. From the nanodiffraction data, real-space maps of the ferroelectric domain structure around the grain boundary prior to and during application of a 200 kV cm −1 electric field were reconstructed. In the vicinity of the tilt grain boundary, the distributions of densities of c -type tetragonal domains with the c axis aligned with the film normal were calculated on the basis of diffracted intensity ratios of c - and a -type domains and reference powder diffraction data. Diffracted intensity was averaged along the grain boundary, and it was shown that the density of c -type tetragonal domains dropped to ∼50% of that of the bulk of the film over a range ±150 nm from the grain boundary. This work complements previous results acquired by band excitation piezoresponse force microscopy, suggesting that reduced nonlinear piezoelectric response around grain boundaries may be related to the change in domain structure, as well as to the possibility of increased pinning of domain wall motion. The implications of the results and analysis in terms of understanding the role of grain boundaries in affecting the nonlinear piezoelectric and dielectric responses of ferroelectric materials are discussed.

36 MATERIALS SCIENCE↗

Linking Domain Structure Evolution at a Grain Boundary to Piezoelectric Response via Nano‐Diffraction

Electric-field-induced domain structure switching in a 1 𝜇⁢m -thick Pb 0.99 (Zr 0.45 Ti 0.55 ) 0.98 Nb 0.02 O 3 (Nb-doped PZT) bicrystal film was characterized in situ via nano-focused synchrotron diffraction. The epitaxial film was deposited on a (100) SrTiO 3 bicrystal substrate. The changes in domain structure were mapped within a 5 𝜇⁢m × 5 𝜇⁢m area at and around an in-plane tilt-type (23.6°) grain boundary with 50 nm spatial resolution. Rocking curves collected at each point of the mapped area provided the ability to reconstruct spatially-varying three-dimensional (3D) reciprocal space maps around the grain boundary. The 3D reciprocal space maps reveal how different tilted 𝑎 -type domain variants interact with the grain boundary as a function of increasing electric field. Initially, a subset of 𝑎 -type domain variants with their polarization vectors largely orthogonal to the grain boundary were found in greater abundance within 570 nm of the grain boundary, possibly due to X-ray beam-induced local increases in the electrical conductivity, but after the coercive field was exceeded, reconfiguration of the ferroelastic domains was observed. The spatially-varying reciprocal space maps also facilitated evaluation of the strain field across the mapped area, along with 𝑑 33,𝑓 . Significant spatial heterogeneity of strain and 𝑑 33,𝑓 are observed, especially at the coercive field, which was attributed to maintaining deformation compatibility and correlated ferroelastic switching.

36 MATERIALS SCIENCE↗

Magnetic domain structure in nanocrystalline Ni-Zn-Co spinel ferrite thin films using off-axis electron holography

We report a study of the magnetic domain structure of nanocrystalline thin films of nickel-zinc ferrite. The ferrite films were synthesized using aqueous spin-spray coating at low temperature (∼90 °C) and showed high complex permeability in the GHz range. Electron microscopy and microanalysis revealed that the films consisted of columnar grains with uniform chemical composition. Off-axis electron holography combined with magnetic force microscopy indicated a multi-grain domain structure with in-plane magnetization. The correlation between the magnetic domain morphology and crystal structure is briefly discussed.

36 MATERIALS SCIENCE↗

Ferroelectric domain structures in <001>-oriented K{sub 0.15}Na{sub 0.85}NbO{sub 3} lead-free single crystal

In this work, ferroelectric domain structures of <001 >-oriented K{sub 0.15}Na{sub 0.85}NbO{sub 3} single crystal are characterized. Transmission electron microscopy (TEM) observation revealed high-density of laminate domain structures in the crystal and the lattices of the neighboring domains are found to be twisted in a small angle. Superlattice diffraction spots of 1/2 (eeo) and 1/2 (ooe) in electron diffraction patterns are observed in the crystal, revealing the a{sup +}a{sup +}c{sup −} tilting of oxygen octahedral in the perovskite structure. The piezoresponse of domains and in-situ poling responses of K{sub 0.15}Na{sub 0.85}NbO{sub 3} crystal are observed by piezoresponse force microscopy (PFM), and the results assure its good ferroelectric properties.

36 MATERIALS SCIENCE↗

Oxyanion Induced Variations in Domain Structure for Amorphous Cobalt Oxide Oxygen Evolving Catalysts, Resolved by X-ray Pair Distribution Function Analysis

Amorphous thin film oxygen evolving catalysts, OECs, of first-row transition metals show promise to serve as self-assembling photoanode materials in solar-driven, photoelectrochemical `artificial leaf' devices. This report demonstrates the ability to use high-energy X-ray scattering and atomic pair distribution function analysis, PDF, to resolve structure in amorphous metal oxide catalyst films. The analysis is applied here to resolve domain structure differences induced by oxyanion substitution during the electrochemical assembly of amorphous cobalt oxide catalyst films, Co-OEC. PDF patterns for Co-OEC films formed using phosphate, Pi, methylphosphate, MPi, and borate, Bi, electrolyte buffers show that the resulting domains vary in size following the sequence Pi < MPi < Bi. The increases in domain size for CoMPi and CoBi were found to be correlated with increases in the contributions from bilayer and trilayer stacked domains having structures intermediate between those of the LiCoOO and CoO(OH) mineral forms. The lattice structures and offset stacking of adjacent layers in the partially stacked CoMPi and CoBi domains were best matched to those in the LiCoOO layered structure. The results demonstrate the ability of PDF analysis to elucidate features of domain size, structure, defect content and mesoscale organization for amorphous metal oxide catalysts that are not readily accessed by other X-ray techniques. Finally, PDF structure analysis is shown to provide a way to characterize domain structures in different forms of amorphous oxide catalysts, and hence provide an opportunity to investigate correlations between domain structure and catalytic activity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Influence of crystallographic orientation and applied magnetic field on domain structure in duplex stainless steel studied using magnetic force microscopy

Highlights: • Ferrite phase in a duplex stainless steel consists of stripe type domains. • Domain contrast decreases with deviation of plane normal from <100>. • Domain width increases with deviation of plane normal from <100>. • Domain alignment with applied field observed along <100> directions. • Grain boundary stray field is a function of misorientation between grains. - Abstract: The paper investigates the local micro-magnetization behavior in duplex stainless steel (DSS) using magnetic force microscopy (MFM). DSS has equal amount of austenite phase in ferrite matrix. The MFM imaging clearly differentiates ferrite phase (ferromagnetic) from the austenite phase (paramagnetic) due to the maze type magnetic domains present in the ferrite phase. The magneto crystalline anisotropic effect on the domain structure is discussed with the support of electron backscatter diffraction (EBSD) measurements. The MFM phase contrast and domain width are correlated with the orientation of surface normal with respect to the easy axis of magnetization (<100>). The influence of external magnetic field (±127 kA/m) application on the domain structure is studied as a function of the grain orientation and the leakage field at the grain boundaries is analyzed based on the mis-orientation between the grains.

36 MATERIALS SCIENCE↗

Experimental observation of the interaction of propagating spin waves with Néel domain walls in a Landau domain structure

The interaction of propagating dipolar spin waves with magnetic domain walls is investigated in square-shaped microstructures patterned from the Heusler compound Co{sub 2}Mn{sub 0.6}Fe{sub 0.4}Si. Using magnetic force microscopy, the reversible preparation of a Landau state with four magnetic domains separated by Néel domain walls is confirmed. A local spin-wave excitation using a microstructured antenna is realized in one of the domains. It is shown by Brillouin light scattering microscopy that the domain structure in the remanence state has a strong influence on the spin-wave excitation and propagation. The domain walls strongly reflect the spin waves and can be used as spin-wave reflectors. A comparison with micromagnetic simulations shows that the strong reflection is due to the long-range dipolar interaction which has important implications for the use of these spin waves for exerting an all-magnonic spin-transfer torque.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗