Search

The tetragonal intermetallic compound EuAl$_{4}$ hosts an exciting variety of low temperature phases. In addition to a charge density wave below 140 K, four ordered magnetic phases are observed below 15.4 K. Recently, a skyrmion phase was proposed based on Hall effect measurements under a $c$-axis magnetic field. We present a detailed investigation of the phase transitions in EuAl$_{4}$ under $c$-axis magnetic field. Our dilatometry, heat capacity, DC magnetometry, AC magnetic susceptibility, and resonant ultrasound spectroscopy measurements reveal three magnetic phase transitions not previously reported. We discuss what our results reveal about the character of the magnetic phases. Our first key result is a detailed $H \parallel [001]$ magnetic phase diagram mapping the seven phases we observe. Second, we identify a new high-field phase, phase VII, which directly corresponds to the region were skyrmions have been suggested. Our results provide guidance for future studies exploring the complex magnetic interactions and spin structures in EuAl$_{4}$., Comment: 20 pages, 15 figures

We report on the impact of magnetoelastic coupling on the magnetocaloric properties of LaFe$_{11.4}$Si$_{1.6}$H$_{1.6}$ in terms of the vibrational density of states, which we determined with $^{57}$Fe nuclear resonant inelastic X-ray scattering measurements and with density-functional-theory based first-principles calculations in the ferromagnetic low-temperature and paramagnetic high-temperature phase. In experiments and calculations, we observe pronounced differences in the shape of the Fe-partial VDOS between non-hydrogenated and hydrogenated samples. This shows that hydrogen does not only shift the temperature of the first-order phase transition, but also affects the elastic response of the Fe-subsystem significantly. In turn, the anomalous redshift of the Fe VDOS, observed by going to the low-volume PM phase, survives hydrogenation. As a consequence, the change in the Fe specific vibrational entropy $\Delta S_\mathrm{lat}$ across the phase transition has the same sign as the magnetic and electronic contribution. DFT calculations show that the same mechanism, which is a consequence of the itinerant electron metamagnetism associated with the Fe subsystem, is effective in both the hydrogenated and he hydrogen-free compounds. Although reduced by 50 % as compared to the hydrogen-free system, the measured change $\Delta S_\mathrm{lat}$ of 3.2\pm1.9 J/kgK across the FM to PM transition contributes with 35 % significantly and cooperatively to the total isothermal entropy change $\Delta S_\mathrm{iso}$. Hydrogenation is observed to induce an overall blueshift of the Fe-VDOS with respect to the H-free compound; this effect, together with the enhanced Debye temperature observed, is a fingerprint of the hardening of the Fe sublattice by hydrogen incorporation. In addition, the mean Debye velocity of sound of LaFe$_{11.4}$Si$_{1.6}$H$_{1.6}$ was determined from the NRIXS and the DFT data., Comment: 13 pages 9 figures

We combine $^{57}$Fe M\"ossbauer spectroscopy and $^{57}$Fe nuclear resonant inelastic x-ray scattering (NRIXS) in nanoscale polycrystalline [bcc-$^{57}$Fe/MgO] multilayers with various Fe layer thicknesses and layer-resolved density-functional-theory (DFT) based first-principles calculations of a (001)-oriented [Fe(8 ML)/MgO(8 ML)](001) heterostructure to unravel the interface-related atomic vibrational properties of a multilayer system. In theory and experiment, we observe consistently enhanced hyperfine magnetic fields compared to bulk which are associated with the Fe/MgO interface layers. NRIXS and DFT both reveal a strong reduction of the longitudinal acoustic (LA) phonon peak in combination with an enhancement of the low-energy vibrational density of states (VDOS) suggesting that the presence of interfaces and the associated increase in the layer-resolved magnetic moments results in drastic changes in the Fe-partial VDOS. From the experimental and calculated VDOS, vibrational thermodynamic properties have been determined as a function of Fe thickness and are found to be in excellent agreement., Comment: 14 pages, 6 figures

BaFe$_2$S$_3$ is a quasi one-dimensional Mott insulator that orders antiferromagnetically below 117(5)\,K. The application of pressure induces a transition to a metallic state, and superconductivity emerges. The evolution of the magnetic behavior on increasing pressure has up to now been either studied indirectly by means of transport measurements, or by using local magnetic probes only in the low pressure region. Here, we investigate the magnetic properties of BaFe$_2$S$_3$ up to 9.9\,GPa by means of synchrotron $^{57}$Fe M\"ossbauer spectroscopy experiments, providing the first local magnetic phase diagram. The magnetic ordering temperature increases up to 185(5) K at 7.5\,GPa, and is fully suppressed at 9.9\,GPa. The low-temperature magnetic hyperfine field is continuously reduced from 12.9 to 10.3\,T between 1.4 and 9.1\,GPa, followed by a sudden drop to zero at 9.9\,GPa indicating a first-order phase transition. The pressure dependence of the magnetic order in BaFe$_2$S$_3$ can be qualitatively explained by a combination of a bandwidth-controlled insulator-metal transition as well as a pressure enhanced exchange interaction between Fe-atoms and Fe 3\textit{d}-S 3\textit{p} hybridization., Comment: 4 pages, 4 figures

We investigated LaFeAsO single crystals by means of synchrotron M\"ossbauer spectroscopy under pressures up to 7.5 GPa and down to 13 K and provide a microscopic phase diagram. We found a continuous suppression of the magnetic hyperfine field with increasing pressure and it completely vanishes at $\sim$ 7.5 GPa which is in contrast to the behavior in polycrystalline samples where the magnetic order vanishes at $\sim$ 20 GPa. The different behavior of the polycrystalline samples might be due to As-vacancies. Our results are in qualitative agreement with density functional theory calculations where a reduction of the magnetic moment with increasing pressure was found. We found that among different samples at ambient pressure the magnetic phase transition temperature as well as the low-temperature magnetic hyperfine field decrease with increasing unit cell volume., Comment: 6 pages, 6 figures

We present a detailed investigation of the electronic properties of CeFeAsO under chemical (As by P substitution) and hydrostatic pressure by means of in-house and synchrotron M\"ossbauer spectroscopy. The Fe magnetism is suppressed due to both pressures and no magnetic order was observed above a P-substitution level of 40% or 5.2 GPa hydrostatic pressure. We compared both pressures and found that the isovalent As by P substitution change the crystallographic and electronic properties differently than hydrostatic pressure., Comment: supplement is included in the pdf file

FeSe, despite being the structurally simplest compound in the family of iron-based superconductors, shows an astoundingly rich interplay of physical phenomena including nematicity and pressure-induced magnetism. Here, we present a microscopic study of these two phenomena by high-energy x-ray diffraction and time-domain M\"ossbauer spectroscopy on FeSe single crystals over a wide temperature and pressure range. The topology of the pressure-temperature phase diagram is a surprisingly close parallel to the well-known doping-temperature phase diagram of BaFe2As2 generated through partial Fe/Co and Ba/Na substitution. In FeSe with pressure p as a control parameter, the magneto-structural ground state can be tuned from "pure" nematic - paramagnetic with an orthorhombic lattice distortion - through a strongly coupled magnetically ordered and orthorhombic state to a magnetically ordered state without an orthorhombic lattice distortion. The magnetic hyperfine field increases monotonically over a wide pressure range. However, the orthorhombic distortion initially decreases under increasing pressure, but is stabilized by cooperative coupling to the pressure-induced magnetic order. Close to the reported maximum of the superconducting critical temperature Tc (occuring at p = 6.8 GPa), the orthorhombic distortion suddenly disappears and FeSe remains tetragonal down to the lowest temperature measured. Analysis of the structural and magnetic order parameters suggests an independent origin of the structural and magnetic ordering phenomena, and their cooperative coupling leads to the similarity with the canonical phase diagram of iron pnictides.

We present phonon dispersions, element-resolved vibrational density of states (VDOS) and corresponding thermodynamic properties obtained by a combination of density functional theory (DFT) and nuclear resonant inelastic X-ray scattering (NRIXS) across the metamagnetic transition of B2 FeRh in the bulk material and thin epitaxial films. We see distinct differences in the VDOS of the antiferromagnetic (AF) and ferromagnetic (FM) phase which provide a microscopic proof of strong spin-phonon coupling in FeRh. The FM VDOS exhibits a particular sensitivity to the slight tetragonal distortions present in epitaxial films, which is not encountered in the AF phase. This results in a notable change in lattice entropy, which is important for the comparison between thin film and bulk results. Our calculations confirm the recently reported lattice instability in the AF phase. The imaginary frequencies at the $X$-point depend critically on the Fe magnetic moment and atomic volume. Analyzing these non vibrational modes leads to the discovery of a stable monoclinic ground state structure which is robustly predicted from DFT but not verified in our thin film experiments. Specific heat, entropy and free energy calculated within the quasiharmonic approximation suggest that the new phase is possibly suppressed because of its relatively smaller lattice entropy. In the bulk phase, lattice degrees of freedom contribute with the same sign and in similar magnitude to the isostructural AF-FM phase transition as the electronic and magnetic subsystems and therefore needs to be included in thermodynamic modeling., Comment: 15 pages, 12 figures

Nuclear resonant inelastic x-ray scattering is used to measure the projected partial phonon density of states of materials. A relationship is derived between the low-energy part of this frequency distribution function and the sound velocity of materials. Our derivation is valid for harmonic solids with Debye-like low-frequency dynamics. This method of sound velocity determination is applied to elemental, composite, and impurity samples which are representative of a wide variety of both crystalline and noncrystalline materials. Advantages and limitations of this method are elucidated.