arXiv subjects

Johanna Lill

Publications and source records attributed to Johanna Lill.

5 recordsLinked to original sources

arXiv2025

Voltage-driven 90 switching of bulk perpendicular magnetic anisotropy in ferrimagnets

Unravelling the mechanism behind bulk perpendicular magnetic anisotropy (PMA) in amorphous rare earth-transition metal films has proven challenging. This is largely due to the inherent complexity of amorphous structure and the entangled potential origins arising from microstructure and atomic structure factors. Here, we present an approach wherein the magneto-electric effect is harnessed to induce 90° switching of bulk PMA in Tb-Co films to in-plane directions by applying voltages of only -1.2 V. This manipulation is achieved by voltage-driven insertion of hydrogen atoms into interstitial sites between Tb and Co atoms, which serves as a perturbation to local atomic structure. Using angle-dependent X-ray magnetic circular dichroism, we find that the anisotropy switching originates from the distortion of crystal field around Tb which reorients the alignment of Tb orbital moments. Initially aligned along Tb-Co bonding directions, the easy magnetization axis undergoes reorientation and switches by 90°, as substantiated by ab-initio calculations. Our study not only concludes the atomic origin of Tb-Co atom bonding configuration in shaping bulk PMA, but also establishes the groundwork for electrically programmable ferrimagnetic spintronics, such as controlling domain wall motion and programming artificial spin textures.

cond-mat.mtrl-sci↗

arXiv2023

Local magnetic and geometric structure in Mn-doped La(Fe,Si)13

Magnetic cooling has the potential to replace conventional gas compression refrigeration. Materials such as La(Fe,Si)$_{13}$ exhibit a sizeable first-order magnetocaloric effect, and it is possible to tailor the phase transition towards room temperature by Mn-H-doping, resulting in a large temperature range for operation. Within this work, we discuss variations of the electronic and lattice structure in La(Fe,Si)$_{13}$ with increasing Mn content utilizing X-ray magnetic circular dichroism (XMCD) and extended X-ray absorption fine structure spectroscopy (EXAFS). While XMCD shows a decrease of the magnetic polarization at the Fe K edge, low-temperature EXAFS measurements indicate increased positional disorder in the La environment that is otherwise absent for Fe and Mn. First-principles calculations link the positional disorder to an enlarged Mn-Si distance -- explaining the increased positional disorder in the La surrounding.

cond-mat.mtrl-sci↗

arXiv2021

Complete crystallographic, spin-electronic and magnetic structure of (Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)3O4: Unraveling the suppression of entropy in high entropy oxides

High entropy oxides (HEOs) are a rapidly emerging class of functional materials consisting of multiple principal cations. The original paradigm of HEOs assumes cationic occupations with the highest possible configurational entropy allowed by the composition and crystallographic structure. However, the fundamental question remains on the actual degree of configurational disorder in HEOs, especially, in systems with a low enthalpy barriers for cation anti-site mixing. Considering the experimental limitations due to the presence of multiple principal cations in HEOs, here we utilize a robust and cross-referenced characterization approach using soft X-ray magnetic circular dichroism, hard X-ray absorption spectroscopy, Mössbauer spectroscopy, neutron powder diffraction and SQUID magnetometry to study the competition between crystal field stabilization energy and configurational entropy governing the cation occupation in a spinel HEO (S-HEO), (Co$_{0.2}$Cr$_{0.2}$Fe$_{0.2}$Mn$_{0.2}$Ni$_{0.2}$)$_3$O$_4$. In contrast to the previous studies, the derived complete structural and spin-electronic model, (Co$_{0.6}$Fe$_{0.4}$)(Cr$_{0.3}$Fe$_{0.1}$Mn$_{0.3}$Ni$_{0.3}$)$_2$O$_4$, highlights a significant deviation from the hitherto assumed paradigm of entropy-driven non-preferential distribution of cations in HEOs. An immediate correlation of this result can be drawn with bulk as well as the local element specific magnetic properties, which are intrinsically dictated by cationic occupations in spinels. The real local lattice picture presented here provides an alternate viewpoint on ionic arrangement in HEOs, which is of fundamental interest for predicting and designing their structure-dependent functionalities.

cond-mat.mtrl-sci↗

arXiv2020

Role of intermediate 4$f$ states in tuning the band structure of high entropy oxides

High entropy oxides (HEOs) are single phase solid solutions consisting of 5 or more cations in approximately equiatomic proportions. In this study, we show reversible control of optical properties in a rare-earth (RE) based HEO-(Ce$_{0.2}$La$_{0.2}$Pr$_{0.2}$Sm$_{0.2}$Y$_{0.2}$)O$_{2-δ}$ and subsequently utilize a combination of spectroscopic techniques to derive the features of the electronic band structure underpinning the observed optical phenomena. Heat treatment of the HEO under vacuum atmosphere followed by reheat-treatment in air results in a reversible change of the band gap energy, from 1.9 eV to 2.5 eV. The finding is consistent with the reversible changes in the oxidation state and related $f$-orbital occupancy of Pr. However, no pertinent changes in the phase composition or crystal structure is observed upon the vacuum heat treatment. Further annealing of this HEO under H$_2$ atmosphere, followed by reheat-treatment in air, results in even larger but still reversible change of the band gap energy from 1.9 eV to 3.2 eV. This is accompanied by a disorder-order type crystal structure transition and changes in the O 2$p$-RE 5$d$ hybridization evidenced from X-ray absorption near edge spectra (XANES). The O $K$ and RE ${M_{4,5}}$/$L_{3}$ XANES indicate that the presence of Ce and Pr (in 3+/4+) state leads to the formation of intermediate 4$f$ energy levels between the O 2$p$ and RE 5$d$ gap in HEO. It is concluded that heat treatment under reducing/oxidizing atmospheres affects these intermediate levels, thus, offering the possibility to tune the band gap energy in HEO.

cond-mat.mtrl-sci↗

arXiv2019

Magnetic response of FeRh to static and dynamic disorder

Changes of the magnetic and crystal structure on the microscopic scale in 40 nm FeRh thin films have been applied to investigate the phenomena of a disorder induced ferromagnetism at room temperature initiated through light ion-irradiation with fluences up to 0.125 Ne$^+$/nm$^{-2}$. Magnetometry shows an increase of magnetic ordering at low temperatures and a decrease of the transition temperature combined with a broadening of the hysteresis with rising ion fluence. $^{57}$Fe Mössbauer spectroscopy reveals the occurrence of an additional magnetic contributions with an hyperfine splitting of 27.2 T - identical to that of ferromagnetic B2-FeRh. The appearance of an anti-site Fe-contribution can be assumed to be lower than 0.6 Fe-at%, indicating that no change of the chemical composition is evident. The investigation of the local structure shows an increase of the static mean square relative displacement determined by X-ray absorption fine structure spectroscopy, while an increase of the defect-concentration has been determined by positron annihilation spectroscopy. From the changes of the microscopic magnetic structure a similarity between the temperature induced and the structural disorder induced ferromagnetic phase can be observed. These findings emphasize the relationship between magnetic ordering and the microscopic defect structure in FeRh.

cond-mat.mtrl-sci↗