Catalyzing capping layers on top of metal hydrides are often employed to enhance the hydrogenation kinetics of metal-hydride based systems such as hydrogen sensors. Here, we experimentally study the hydrogenation kinetics of capping layers composed o
f several alloys of Pd and Au as well as Pt, Ni and Ru, all with and without an additional PTFE protection layer using a novel method and under the same set of experimental conditions. Our results demonstrate that doping Pd with Au results in significantly faster hydrogenation kinetics, with response times up to five times shorter than Pd through enhanced diffusion and a reduction of the activation energy. The kinetics of non-Pd based materials turns out to be significantly slower and mainly limited by the diffusion through the capping layer itself. Surprisingly, the additional PTFE layer was only found to improve the kinetics of Pd-based capping materials and has no significant effect on the kinetics of Pt, Ni and Ru. Taken together, the experimental results aid in rationally choosing a suitable capping material for the application of metal hydrides and other materials in a green economy. In addition, the developed method can be used to simultaneously study the hydrogenation kinetics and determine diffusion constants in thin film materials for a wide set of experimental conditions.
Hydrogen detection in a reliable, fast, and cost-effective manner is a prerequisite for the large-scale implementation of hydrogen in a green economy. We present thin film Ta$_{1-y}$Pd$_y$ as effective optical sensing materials with extremely wide se
nsing ranges covering at least seven orders of magnitude in hydrogen pressure. Nanoconfinement of the Ta$_{1-y}$Pd$_y$ layer suppresses the first-order phase transitions present in bulk and ensures a sensing response free of any hysteresis. Unlike other sensing materials, Ta$_{1-y}$Pd$_y$ features the special property that the sensing range can be easily tuned by varying the Pd concentration without a reduction of the sensitivity of the sensing material. Combined with a suitable capping layer, sub-second response times can be achieved even at room temperature, faster than any other known thin-film hydrogen sensor.
The archetype cubic chiral magnet MnSi is home to some of the most fascinating states in condensed matter such as skyrmions and a non-Fermi liquid behavior in conjunction with a topological Hall effect under hydrostatic pressure. Using small angle ne
utron scattering, we study the evolution of the helimagnetic, conical and skyrmionic correlations with increasing hydrostatic pressure. We show that the helical propagation vector smoothly reorients from $langle 111 rangle$ to $langle100rangle$ at intermediate pressures. At higher pressures, above the critical pressure, the long-range helimagnetic order disappears at zero magnetic field. Nevertheless, skyrmion lattices and conical spirals form under magnetic fields, in a part of the phase diagram where a topological Hall effect and a non-Fermi liquid behavior have been reported. These unexpected results shed light on the puzzling behavior of MnSi at high pressures and the mechanisms that destabilize the helimagnetic long-range order at the critical pressure.
We present a comprehensive small angle neutron scattering study of the doping dependence of the helimagnetic correlations in Mn$_{1-x}$Fe$_{x}$Si. The long-range helimagnetic order in Mn$_{1-x}$Fe$_x$Si is suppressed with increasing Fe content and di
sappears for $x$ $>$ $x^*$ $approx$ 0.11, i.e. well before $x_C$ $approx$ 0.17 where the transition temperature vanishes. For $x$ $>$ $x^*$, only finite isotropic helimagnetic correlations persist which bear similarities with the magnetic correlations found in the precursor phase of MnSi. Magnetic fields gradually suppress and partly align these short-ranged helimagnetic correlations along their direction through a complex magnetization process.
We present a comprehensive and systematic magnetization and ac susceptibility study of Mn$_{1-x}$Fe$_{x}$Si over an extensive range of ten Fe concentrations between $x$ = 0 - 0.32. With increasing Fe substitution, the critical temperature decreases b
ut the magnetic phase diagrams remain qualitatively unaltered for $x$ $leq$ $x^*$ $approx$ 0.11 with clear boundaries between the helical, conical, and skyrmion lattice phase as well as an enhanced precursor phase. A notably different behavior sets in for $x$ $=$ 0.11, 0.13 and 0.14, where certain characteristics of helimagnetic correlations persist, but without clear phase boundaries. Although a qualitative change already sets in at $x^*$, the transition temperature and spontaneous magnetization vanish only at $x_C$ = 0.17 where also the average magnetic interactions change sign. Although the Curie-Weiss temperature reaches -12~K for $x$ = 0.32, no signature of long-range magnetic order is found down to the lowest temperature, indicating a possible significant role for quantum fluctuations in these systems.
Magnetic skyrmions are nano-sized topologically protected spin textures with particle-like properties. They can form lattices perpendicular to the magnetic field and the orientation of these skyrmion lattices with respect to the crystallographic latt
ice is governed by spin-orbit coupling. By performing small angle neutron scattering measurements, we investigate the coupling between the crystallographic and skyrmion lattices in both Cu$_2$OSeO$_3$ and the archetype chiral magnet MnSi. The results reveal that the orientation of the skyrmion lattice is primarily determined by the magnetic field direction with respect to the crystallographic lattice. In addition, it is also influenced by the magnetic history of the sample which can induce metastable lattices. Kinetic measurements show that these metastable skyrmion lattices may or may not relax to their equilibrium positions under macroscopic relaxation times. Furthermore, multidomain lattices may form when two or more equivalent crystallographic directions are favored by spin-orbit coupling and oriented perpendicular to the magnetic field.
We present a comprehensive Small Angle Neutron Scattering (SANS) and Neutron Spin Echo Spectroscopy (NSE) study of the structural and dynamical aspects of the helimagnetic transition in Fe$_{1-x}$Co$_x$Si with $x$ = 0.30. In contrast to the sharp tra
nsition observed in the archetype chiral magnet MnSi, the transition in Fe$_{1-x}$Co$_x$Si is gradual and long-range helimagnetic ordering coexists with short-range correlations over a wide temperature range. The dynamics are more complex than in MnSi and involve long relaxation times with a stretched exponential relaxation which persists even under magnetic field. These results in conjunction with an analysis of the hierarchy of the relevant length scales show that the helimagnetic transition in Fe$_{1-x}$Co$_x$Si differs substantially from the transition in MnSi and question the validity of a universal approach to the helimagnetic transition in chiral magnets.
Small angle neutron scattering measurements on a bulk single crystal of the doped chiral magnet Fe$_{1-x}$Co$_x$Si with $x$=0.3 reveal a pronounced effect of the magnetic history and cooling rates on the magnetic phase diagram. The extracted phase di
agrams are qualitatively different for zero and field cooling and reveal a metastable skyrmion lattice phase outside the A-phase for the latter case. These thermodynamically metastable skyrmion lattice correlations coexist with the conical phase and can be enhanced by increasing the cooling rate. They appear in a wide region of the phase diagram at temperatures below the $A$-phase but also at fields considerably smaller or higher than the fields required to stabilize the A-phase.
We present a systematic study of the ac susceptibility of the chiral magnet Fe$_{1-x}$Co$_x$Si with $x$ = 0.30 covering four orders of magnitude in frequencies from 0.1 Hz to 1 kHz, with particular emphasis to the pronounced history dependence. Chara
cteristic relaxation times ranging from a few milliseconds to tens of seconds are observed around the skyrmion lattice A-phase, the helical-to-conical transition and in a region above $T_C$. The distribution of relaxation frequencies around the A-phase is broad, asymmetric and originates from multiple coexisting relaxation processes. The pronounced dependence of the magnetic phase diagram on the magnetic history and cooling rates as well as the asymmetric frequency dependence and slow dynamics suggest more complicated physical phenomena in Fe$_{0.7}$Co$_{0.3}$Si than in other chiral magnets.
The reference chiral helimagnet MnSi is the first system where skyrmion lattice correlations have been reported. At zero magnetic field the transition at $T_C$ to the helimagnetic state is of first order. Above $T_C$, in a region dominated by precurs
or phenomena, neutron scattering shows the build up of strong chiral fluctuating correlations over the surface of a sphere with radius $2pi/ell$, where $ell$ is the pitch of the helix. It has been suggested that these fluctuating correlations drive the helical transition to first order following a scenario proposed by Brazovskii for liquid crystals. We present a comprehensive neutron scattering study under magnetic fields, which provides evidence that this is not the case. The sharp first order transition persists for magnetic fields up to 0.4 T whereas the fluctuating correlations weaken and start to concentrate along the field direction already above 0.2 T. Our results thus disconnect the first order nature of the transition from the precursor fluctuating correlations. They also show no indication for a tricritical point, where the first order transition crosses over to second order with increasing magnetic field. In this light, the nature of the first order helical transition and the precursor phenomena above $T_C$, both of general relevance to chiral magnetism, remain an open question.
