Kornelius Nielsch

Reducing the nucleation barrier in magnetocaloric Heusler alloys by nanoindentation

Magnetocaloric materials are promising as solid state refrigerants for more efficient and environmentally friendly cooling devices. The highest effects have been observed in materials that exhibit a first-order phase transition. These transformations proceed by nucleation and growth which lead to a hysteresis. Such irreversible processes are undesired since they heat up the material and reduce the efficiency of any cooling application. In this article, we demonstrate an approach to decrease the hysteresis by locally changing the nucleation barrier. We created artificial nucleation sites and analyzed the nucleation and growth processes in their proximity. We use Ni-Mn-Ga, a shape memory alloy that exhibits a martensitic transformation. Epitaxial films serve as a model system, but their high surface-to-volume ratio also allows for a fast heat transfer which is beneficial for a magnetocaloric regenerator geometry. Nanoindentation is used to create a well-defined defect. We quantify the austenite phase fracti...

Atom size electron vortex beams with selectable orbital angular momentum

The decreasing size of modern functional magnetic materials and devices cause a steadily increasing demand for high resolution quantitative magnetic characterization. Transmission electron microscopy (TEM) based measurements of the electron energy-loss magnetic chiral dichroism (EMCD) may serve as the needed experimental tool. To this end, we present a reliable and robust electron-optical setup that generates and controls user-selectable single state electron vortex beams with defined orbital angular momenta. Our set-up is based on a standard high-resolution scanning TEM with probe aberration corrector, to which we added a vortex generating fork aperture and a miniaturized aperture for vortex selection. We demonstrate that atom size probes can be formed from these electron vortices and that they can be used for atomic resolution structural and spectroscopic imaging – both of which are prerequisites for future atomic EMCD investigations.

Nucleation and growth of hierarchical martensite in epitaxial shape memory films

Abstract Shape memory alloys often show a complex hierarchical morphology in the martensitic state. To understand the formation of this twin-within-twins microstructure, we examine epitaxial Ni-Mn-Ga films as a model system. In-situ scanning electron microscopy experiments show beautiful complex twinning patterns with a number of different mesoscopic and macroscopic twin boundaries between already twinned regions. We explain the appearance and geometry of these patterns by constructing an internally twinned martensitic nucleus, which can take the shape of a diamond or a parallelogram, within the basic phenomenological theory of martensite. These nucleus contains already the seeds of different possible mesoscopic twin boundaries. Nucleation and growth of these nuclei determines the creation of the hierarchical space-filling martensitic microstructure. This is in contrast to previous approaches to explain a hierarchical martensitic microstructure. This new picture of creation and anisotropic, well-oriented growth of twinned martensitic nuclei explains the morphology and exact geometrical features of our experimentally observed twins-within-twins microstructure on the meso- and macroscopic scale.

Research Update: Magnetoionic control of magnetization and anisotropy in layered oxide/metal heterostructures

Electric field control of magnetization and anisotropy in layered structures with perpendicular magnetic anisotropy is expected to increase the versatility of spintronic devices. As a model system for reversible voltage induced changes of magnetism by magnetoionic effects, we present several oxide/metal heterostructures polarized in an electrolyte. Room temperature magnetization of Fe-O/Fe layers can be changed by 64% when applying only a few volts in 1M KOH. In a next step, the bottom interface of the in-plane magnetized Fe layer is functionalized by an L10 FePt(001) underlayer exhibiting perpendicular magnetic anisotropy. During subsequent electrocrystallization and electrooxidation, well defined epitaxial Fe3O4/Fe/FePt heterostructures evolve. The application of different voltages leads to a thickness change of the Fe layer sandwiched between Fe-O and FePt. At the point of transition between rigid magnet and exchange spring magnet regime for the Fe/FePt bilayer, this induces a large variation of magnet...

Modulations in martensitic Heusler alloys originate from nanotwin ordering

Heusler alloys exhibiting magnetic and martensitic transitions enable applications like magnetocaloric refrigeration and actuation based on the magnetic shape memory effect. Their outstanding functional properties depend on low hysteresis losses and low actuation fields. These are only achieved if the atomic positions deviate from a tetragonal lattice by periodic displacements. The origin of the so-called modulated structures is the subject of much controversy: They are either explained by phonon softening or adaptive nanotwinning. Here we used large-scale density functional theory calculations on the Ni2MnGa prototype system to demonstrate interaction energy between twin boundaries. Minimizing the interaction energy resulted in the experimentally observed ordered modulations at the atomic scale, it explained that a/b twin boundaries are stacking faults at the mesoscale, and contributed to the macroscopic hysteresis losses. Furthermore, we found that phonon softening paves the transformation path towards the nanotwinned martensite state. This unified both opposing concepts to explain modulated martensite.

Superconducting properties of Ba(Fe1- xNix)2As2 thin films in high magnetic fields

We report on the electrical transport properties of epitaxial Ba(Fe1–xNix)2As2 thin films grown by pulsed laser deposition in static magnetic fields up to 35 T. The thin film shows a critical temperature of 17.2 K and a critical current density of 5.7 × 105 A/cm2 in self field at 4.2 K, while the pinning is dominated by elastic pinning at two-dimensional nonmagnetic defects. Compared to the single-crystal data, we find a higher slope of the upper critical field for the thin film at a similar doping level and a small anisotropy. Also, an unusual small vortex liquid phase was observed at low temperatures, which is a striking difference to Co-doped BaFe2As2 thin films.

Structural and ferroelectric properties of epitaxial BaZr x Ti1−x O3 thin films

Epitaxial BaZr x Ti1−x O3 (BZTO) thin films with Zr contents of x = 0, x = 0.12 and x = 0.2 were grown by pulsed laser deposition on (0 0 1)-oriented single crystalline SrTiO3 substrates utilizing an additional conducting SrRuO3 buffer layer. It was found that the oxygen pressure during the deposition heavily influences the lattice constants and the microstructure of BZTO. A low of 0.01 mbar gives rise to a significant tetragonal distortion. Texture measurements reveal that an undisturbed epitaxial growth is only achieved for BZTO films prepared in 0.01 mbar oxygen. In contrast, the formation of twins was observed for higher . A detailed microstructural analysis indicates that the sample preparation in low prevents a preferential growth of columnar grains within the BZTO layers and leads to smoother film surfaces. BZTO thin films deposited with optimized deposition parameters show characteristic ferroelectric polarization behavior. The saturation polarization at room temperature declines with increasing Zr content and the characteristic ferroelectric hysteresis diminishes. Temperature-depended measurements of the relative permittivity reveal the existence of a broad transition range and a significant shift of the phase transition temperature to lower values for increasing Zr content.

Influence of the polarization anisotropy on the electrocaloric effect in epitaxial PMN-PT thin films

Pb(Mg1/3Nb2/3)O3-PbTiO3 (PMN-PT) compounds, which are typically used for high performance actuator applications due to their outstanding piezoelectric properties, show, in addition, a pronounced electrocaloric (EC) effect. The study of epitaxial films is a useful tool to analyze the correlation between the microstructure and EC properties in order to optimize the performance of these materials. Therefore, the 0.9PMN-0.1PT films were grown by a pulsed laser deposition on (001) as well as (111) oriented SrTiO3 single crystalline substrates using a La0.7Sr0.3CoO3 buffer as the bottom electrode and additional Au top electrodes. The structural properties determined by a high resolution X-ray and electron microscopy techniques indicated an undisturbed epitaxial growth. The anisotropy of the ferroelectric domain structure was investigated by a vertical and lateral piezoresponse force microscopy showing clear differences between the two orientations. A significant reduction of the thermal hysteresis was observed ...

Reversible tuning of magnetocaloric Ni-Mn-Ga-Co films on ferroelectric PMN-PT substrates

Tuning functional properties of thin caloric films by mechanical stress is currently of high interest. In particular, a controllable magnetisation or transition temperature is desired for improved usability in magnetocaloric devices. Here, we present results of epitaxial magnetocaloric Ni-Mn-Ga-Co thin films on ferroelectric Pb(Mg1/3Nb2/3)0.72Ti0.28O3 (PMN-PT) substrates. Utilizing X-ray diffraction measurements, we demonstrate that the strain induced in the substrate by application of an electric field can be transferred to the thin film, resulting in a change of the lattice parameters. We examined the consequences of this strain on the magnetic properties of the thin film by temperature- and electric field-dependent measurements. We did not observe a change of martensitic transformation temperature but a reversible change of magnetisation within the austenitic state, which we attribute to the intrinsic magnetic instability of this metamagnetic Heusler alloy. We demonstrate an electric field-controlled entropy change of about 31 % of the magnetocaloric effect - without any hysteresis.

All-electrochemical voltage-control of magnetization in metal oxide/metal nanoislands

The great prospects for low-power magnetoelectronic devices trigger significant research activity aiming at voltage-control of magnetism. In this field, ion migration and reversible electrochemical reactions currently open a pathway to voltage-reprogrammable magnetic materials. Up to now, such electrochemical manipulation of oxide/metal heterostructures is mainly reported for thin films prepared by physical methods. The present study describes an all-electrochemical route by utilizing electrodeposited FeOx/Fe nanoislands as a starting state. Repeatable electrochemical conversion between ferromagnetic Fe and FeOx is achieved in KOH solution and exploited for voltage control of the magnetization of the nanoislands. For the smallest nanoislands, exhibiting dimensions of a few nanometers, almost complete voltage-induced ON/OFF switching of magnetism at room temperature is detected by in situ transport and ferromagnetic resonance measurements. The observed effects are enhanced in comparison to those of continuous films, which points at the morphology as an influencing factor of electrochemical voltage control of magnetism. The all-electrochemical approach is decisive for extending the application possibilities for voltage-programmable magnetic materials, because, by electrochemical deposition, geometry restrictions can be overcome and 3D structures can be functionalized.