Melting of a skyrmion lattice to a skyrmion liquid via a hexatic phase

While in 3D materials melting is a single, first-order phase transition, in 2D systems, it can also proceed via an intermediate phase. For a skyrmion lattice in Cu2OSeO3, magnetic field variations can tune this quasiparticle 2D solid into a skyrmion liquid via an intermediate hexatic phase with short-range translational and quasi-long-range orientational order. The phase transition most commonly observed is probably melting, a transition from ordered crystalline solids to disordered isotropic liquids. In three dimensions, melting is a single, first-order phase transition. In two-dimensional systems, however, theory predicts a general scenario of two continuous phase transitions separated by an intermediate, oriented liquid state, the so-called hexatic phase with short-range translational and quasi-long-range orientational orders. Such hexatic phases occur in colloidal systems, Wigner solids and liquid crystals, all composed of real-matter particles. In contrast, skyrmions are countable soliton configurations with non-trivial topology and these quasi-particles can form two-dimensional lattices. Here we show, by direct imaging with cryo-Lorentz transmission electron microscopy, that magnetic field variations can tune the phase of the skyrmion ensembles in Cu(2)OSeO(3)from a two-dimensional solid through the long-speculated skyrmion hexatic phase to a liquid. The local spin order persists throughout the process. Remarkably, our quantitative analysis demonstrates that the aforementioned topological-defect-induced crystal melting scenario well describes the observed phase transitions.

Skyrmion Control and Phase Transitions in Cu2OSeO3

Thomas Schönenberger

Magnetic skyrmions are nanometric and non-trivial spin textures with non-zero topological charge. Their robustness against perturbations and the possibility to control them using external stimuli make them ideal candidates for future spintronic applications. In particular the magnetoelectric skyrmion host Cu2OSeO3 holds a lot of promise for low power devices since skyrmions in this compound can be controlled by electric fields alone. Using Lorentz transmission electron microscopy to perform real space and real time biasing experiments on thin lamellas of Cu2OSeO3 in a geometry that is most suitable for technological applications, we observe reproducible creation and annihilation of skyrmions. For a more quantitative analysis, we develop new feature detection algorithms to reliably extract skyrmion positions even in noisy images. We further produce Due to its low pinning, Cu2OSeO3 allows for the formation of large and well-arranged triangular skyrmion lattices. This makes this compound a perfect testbed to study the evolution of skyrmion configurations under external stimuli. Experiments are carried out again using Lorentz transmission electron microscopy on thin lamellas of Cu2OSeO3. We investigate how defects in skyrmion lattices are arranged at grain boundaries and develop algorithms to extract them and to directly visualize their alignment. These defects are at the core of the melting of skyrmion lattices in this system. We show that a controlled magnetic field ramp can induce skyrmion ensembles in Cu2OSeO3 to transition from a two-dimensional solid through a thus far unknown ordered liquid phase called the hexatic phase, to a liquid. We find that this transition is a topological defect-induced two-step process as predicted by the Kosterlitz-Thouless-Halperin-Nelson-Young (KTHNY) theory. Finally, we go beyond equilibrium phenomena to explore the effect of quenching the system from its liquid phase to its solid phase using different quench rates and find first evidence that our system belongs to the Kibble-Zurek universality class.

EPFL2022

Pulsed laser deposition of (SrBa)Nb2O6 thin films and their properties

Anna Infortuna

Strontium barium niobate (SrxBa1-xNb2O6, shortly SBN) is a solid solution system with tetragonal tungsten bronze crystal structure. It exhibits a ferroelectric phase with only one polar axis and a transition temperature depending on the Sr/Ba ratio. This thesis studies the growth of SBN thin films, in order to obtain a ferroelectric thin film model system for the study of 180° domain switching close to the ferroelectric phase transition. SBN has been chosen not only because uniaxial, but because it is possible to tune the temperature of phase transition varying the Sr/Ba ratio. It is thus possible to study electric properties of the phase transition close to room temperature, where conduction phenomena related to defects are normally lower. Thin films of SBN were grown by Pulsed Laser Deposition in a vacuum system constructed during this thesis work. For the formulation of a model it is desirable to have a system as close as possible to a single crystal. Therefore deposition parameters have been optimized to grow SBN thin films with the polar axis oriented perpendicular to the film plane. The films are integrated in parallel plate capacitor structures, in order to measure dielectric properties. The stability of the ferroelectric phase is found to be sensitive to impurities; contaminants with concentration below 1% induce a lowering of the transition temperature of about 100°C. Strain as well has influence on the phase transition; in the case of substrate with thermal expansion coefficients different from the SBN ones, the SBN film is under stress. A 0.6% tensile strain induces a lowering of the transition temperature of about 100°C, this is the case of silicon single crystal substrate. Grown on strontium titanate single crystals (STO), whose thermo-mechanical properties are close to the one of SBN, the films exhibit a phase transition temperature compatible with the one measured on single crystals. The obtained films suffer from leakage that is reduced by thermal treatment in oxygen rich atmosphere. The oxygen vacancies, created during the deposition process, are considered to be responsible of leakage. Vacancies recovery upon annealing does not eliminate the problem, and measurement of polarization at room temperature is difficult. However, piezoelectric measurements performed on individual grains, with atomic force microscope, prove that these have ferroelectric properties; by these experiment has been proved that it is possible to switch the polarization. Films with a disordered structure of grains are much less leaky than the ones with columnar grains spanning the whole cross section. These observations lead to the conclusion that conduction goes trough the grain boundaries. On STO single crystals, SBN grows epitaxial in Volmer-Weber mode. With a suitable preparation of the substrate surface, it is possible to induce the growth of films with different orientations of the polar axis: in the film plane, perpendicular to it or inclined of 45°. A model is proposed, explaining the epitaxial relation with the substrate on the basis of the perovskite kernel contained in the unit cell of the tetragonal tungsten bronze structure. The film grows from the nucleation of the perovskite structure that rules the orientation of the film; the high temperature at which the substrate is kept during the deposition, assure the necessary mobility for the arriving atoms to organize in the SBN structure around these nuclei. The study of literature data allows to state that such a model is valid not only for substrates with perovskite structure, but can be extended to substrates with a cubic crystal structure, like magnesium oxide.

EPFL2005

Etude par microscopie électronique à transmission à haute résolution de l'élargissement thermique des parois de domaines ferroélectriques dans un système de premier ordre

The macroscopic properties of ferroelectric materials depend directly on the domain configuration and the structure of the domain boundaries. For this reason, their study is of great scientific and technological interest. Several models have been developed to describe the properties of domain walls (structure, thickness, stress at the interface, mobility, …). However, few quantitative experimental observations of ferroelectric domain walls at an atomic scale have been reported, and even less results exist at higher temperatures. The ferroelectric domain-wall thickness is an important parameter whose behavior as a function of temperature is directly related to the order of the phase transition. In a second-order system, the temperature dependence of the domain-wall thickness follows a power law L ~ (Tc - T)-ω where ω is the critical exponent characterizing the divergence of L near the critical temperature Tc The predictions concerning the numerical value of are different depending on the theoretical model considered. Nevertheless, the majority of ferroelectric materials are known to undergo a first-order transition. In these systems the domain-wall thickness increases when the transition temperature is approached, but without diverging as for a second-order phase transition. The major objective of this work was to measure this broadening predicted by the theory for the first time at the approach of the phase transition temperature. We have shown that high resolution transmission electron microscopy is powerful technique for the study of ferroelectric domain walls not only at room temperature but also at higher temperatures. This method allows a direct and local observation of interfaces at an atomic scale which is a considerable advantage over diffraction techniques (X-ray, neutron, electron) and most of the other electron microscopy methods. However, the requirements of this method concerning the performance of the optical system of the microscope, the quality of the specimen and its stability in the column are very high, and today high resolution microscopy at high temperature remains a major challenge. The domain-wall thickness is obtained from the measurement of the crystal lattice distortion near the interface using two different numerical techniques of image analysis. The first method is based on the accurate determination of the center of bright peaks which appear on high resolution images for a judicious choice of the experimental parameters (delocalization and crystal thickness) and which represent the crystal lattice nodes. The second technique consists in selecting a circular region of the power spectrum around a reflection peak, centering the Fourier space on this reflection and performing the inverse Fourier transform. The information about the local displacement of atomic planes corresponding to the selected reflection is extracted form the phase component of the obtained complex image. Both techniques have been successfully applied to the measurement of the thickness of the 90° ferroelectric domain walls in PbTiO3 single crystals. This perovskite presents a first order phase transition at Tc = 492.2°C. which corresponds to the transformation of the crystal from the high-temperature paraelectric cubic phase to the low-temperature ferroelectric tetragonal phase. For the first time, the thermal broadening of domain walls has been measured quantitatively using HRTEM. The results are compared with the predictions made by phenomenological theories. We find that the domain wall thickness increases continuously from 0.7 nm at room temperature up to 5.5 nm near the transition temperature. Our results are consistent with those obtained by other authors at room temperature and those of a very recent study performed at higher temperatures using weak-beam microscopy. The measured domain-wall broadening is greater than the one predicted by a three-dimensional Ginzburg-Landau model where the polarization which is the primary order parameter is coupled to the elastic strain which plays the role of secondary order parameter. Our results are better described by a one-dimensional Ginzburg-Landau model without secondary order parameter. In this case the gradient coupling coefficient κ of the Ginzburg-Landau free energy is found to be 1.3 · 10-10 m3F-1. The methods developed for the measurement of the domain-wall thickness can by applied not only to other first-order ferroelectric crystals but also to ferroelectric systems presenting a second-order phase transition thus allowing the determination of the critical exponent ω. Characteristics only present in 2-D systems could also be detected by studying very thin specimens. Moreover, the same techniques can be adapted to the study of domain walls in purely ferroelastic materials.

EPFL2000