Vojtěch Uhlíř

Even on the nanoscale, phase transitions are governed by both intrinsic and extrinsic heterogeneities, yet capturing their spatio-temporal dynamics remains a challenge. While ultrafast techniques track phase changes on femtosecond timescales, the spatial complexity and stochastic nature of the processes often remain hidden. Here, we present an experimental approach that combines established ultrafast hard-X-ray diffraction with a propagating strain pulse as a universal and non-invasive structural marker. This ultrafast X-ray sonography identifies the spatio-temporal structural phase heterogeneity on nanometer length- and picosecond time-scales by tracking the phase-specific strain response. It offers a versatile platform for investigating a wide range of phase transitions accompanied by structural changes in typical nanometer-thin films. We apply this approach to the antiferromagnetic-to-ferromagnetic magneto-structural phase transition in FeRh. Modeling the phase-specific strain response identifies the nucleation of domains of approximately 20 nm height exhibiting the structural signatures of the ferromagnetic phase.

Electron magnetic circular dichroism (EMCD) in transmission electron microscopy (TEM) enables element-specific measurement of spin and orbital magnetic moments, analogous to x-ray magnetic circular dichroism (XMCD). While the EMCD technique offers unmatched spatial resolution, its quantitative accuracy remains under scrutiny, particularly in beam-splitter geometries with convergent probes. Here, we systematically evaluate the limits of quantitative EMCD analysis using the first-order magnetostructural transition in the functional phase-change material FeRh as a tunable magnetic reference. Unlike previous EMCD studies primarily focused on elemental ferromagnets such as Fe, we demonstrate its applicability to a correlated material exhibiting coupled structural and magnetic order. We demonstrate that the extracted orbital-to-spin moment ratio ( m L / m S ) remains within the same order of magnitude as XMCD benchmarks, despite a systematic reduction in absolute value, for TEM probes down to approximately 6 nm, thereby establishing the validity range for reliable quantification. For nanometer-sized probes with higher convergence angles, we observe an enhanced m L / m S , which we attribute to a combination of instrumental factors and sensitivity to nanoscale heterogeneity within the probed volume. Our results confirm that EMCD provides quantitative agreement with macroscale techniques under suitable conditions, while uniquely enabling spatially confined measurements of local magnetic moments in functional magnetic materials, and allowing the study of interfacial, defect-mediated, or phase-separated magnetism that is inaccessible to photon-based methods.

Controlling magnetic order on ultrafast timescales, driven by spintronic and recording applications, is one of the main directions of current research in magnetism. Despite major advances in understanding the temporal evolution of magnetic order upon its emergence or quenching, experimental demonstration of the local link between microstructure and dynamic nucleation is missing. Here, taking advantage of the high structural and magnetic resolution of transmission electron microscopy, we observe that cumulative laser irradiation significantly alters the nucleation pathway of the first-order antiferromagnetic to ferromagnetic phase transition of FeRh thin films, causing the transition to switch from homogeneous to heterogeneous nucleation. This leads to a decrease of 20 K in transition temperature and the emergence of submicron magnetic vortices as preferential nucleation motifs. These vortices are pinned in the film by underlying dislocation networks. We observe that the dislocation networks are formed and rearranged upon repeated crossing of the phase transition using both femtosecond and picosecond laser pulses. Our results establish a direct link between defect formation and the microscopic morphology of the nucleated ferromagnetic phase, with broad implications for ultrafast stroboscopic experiments and defect-mediated phase transitions in functional materials.

The optical excitation of metals initially creates short-lived non-Fermi distributions of the electrons. The electrons and holes excited far above and below the Fermi level quickly relax to hot Fermi-distributions that subsequently cool via electron-phonon scattering. Here, we show that such non-thermal charge carriers beyond the Fermi-distribution speed up the prototypical first-order antiferromagnetic-to-ferromagnetic phase transition in FeRh. In ultrafast x-ray diffraction experiments, we vary the maximum electron temperature by increasing the pump pulse duration up to 10 ps. For direct optical excitation of FeRh, ferromagnetic domains nucleate within 8 ps as soon as the successively deposited energy surpasses the site-specific threshold energy. In contrast, suppressing the direct optical excitation by an optically opaque Pt layer leads to a nucleation on a 50 ps timescale driven by the near-equilibrium heat transport. These findings unambiguously identify the photo-excitation of non-thermal electrons and not electron-phonon non-equilibria to enable the rapid phase transition in FeRh.

Metamaterials with engineered structures have been extensively investigated for their capability to manipulate optical, acoustic, or thermal waves. In particular, magnetic metamaterials with precise geometry, shape, size and arrangement of their elemental blocks may be used to concentrate, focus, or guide magnetic fields. In this work, we show the potential of using soft-magnetic permalloy (Py) metasurfaces to tailor the physical properties of other magnetic structures at the local scale. As an illustration, the magnetic response of a Cobalt (Co) sensor bar placed at the core of a Py metasurface is investigated as a function of in-plane magnetic fields through the planar Hall effect. Our findings reveal that by appropriately selecting the metasurface geometrical parameters, we can adjust the Co bar's coercive field and susceptibility, leading to a huge enhancement in sensor sensitivity of over 2 orders of magnitude. Micromagnetic simulations, coupled with magneto-transport equations and X-ray photoemission electron measurements (XPEEM) with contrast from magnetic circular dichroism (XMCD), accurately capture this effect and provide insights into the underlying physical mechanisms. These findings can potentially enhance the performance and versatility of magnetic functional devices by using specifically designed structural magnetic materials.

In a step towards generating switchable MRI cellular labels, we demonstrate in-situ field switching of micron scale metamagnetic Iron-Rhodium (FeRh) thin film particles. A thin-film (200 nm) FeRh sample was fabricated and patterned into an array of progressively smaller squares with sizes ranging from 500 μm down to 1 μm. The large first order phase change from antiferromagnetic to ferromagnetic state was characterized using vibrating sample magnetometry, magnetic force microscopy, and MRI. Room temperature MRI experiments sensitive to the local magnetic field surrounding the particles demonstrated the low moment state (OFF MRI contrast) at 4.7T and high moment state (ON MRI contrast) at 11.7T for the array where sizes down to 2–3 μm were observed in MRI at 50 μm resolution. The expected temperature dependent MRI contrast change was seen at 4.7T, where 10 μm particles could be observed at 150 μm resolution in the ON state. A shielded MRI insert, used to temporarily increase or decrease the magnetic field up to 0.77T amplitude, was used to reversibly switch the particle array at constant temperature and blink the particles ON and OFF at 4.7T. This work demonstrates the MRI contrast switching potential for FeRh particles with biological cell dimensions, and the use of magnetic field pulses for reversible MRI label contrast control.

We use ultrafast x-ray diffraction to study non-equilibrium pathways of the phase transition in FeRh parametrized by the structural response. By increasing the pump-pulse duration beyond the electron-phonon coupling time, we suppress the electron-phonon non-equilibrium present upon femtosecond laser excitation but still photoexcite electrons to non-thermal states. Irrespective of the pump pulse duration, we find an optically induced nucleation of ferromagnetic domains on an 8 ps timescale that starts as soon as the successively deposited energy surpasses the site-specific threshold energy. If in contrast, FeRh is only indirectly excited by diffusion of thermalized electrons from an opaque Pt cap layer, the ferromagnetic phase rises on a 50 ps timescale. These findings unambiguously identify the photo-excitation of non-thermal electrons and not electron-phonon non-equilibria to enable the non-equilibrium pathway of the phase transition in FeRh.