Laser-Rewriteable Ferromagnetism at Thin-Film Surfaces.

Manipulation of magnetism using laser light is considered as a key to the advancement of data storage technologies. Until now, most approaches seek to optically switch the direction of magnetization rather than to reversibly manipulate the ferromagnetism itself. Here, we use ∼100 fs laser pulses to reversibly switch ferromagnetic ordering on and off by exploiting a chemical order-disorder phase transition in Fe60Al40, from the B2 to the A2 structure and vice versa. A single laser pulse above a threshold fluence causes nonferromagnetic B2 Fe60Al40 to disorder and form the ferromagnetic A2 structure. Subsequent laser pulsing below the threshold reverses the surface to B2 Fe60Al40, erasing the laser-induced ferromagnetism. Simulations reveal that the order-disorder transition is regulated by the extent of surface supercooling; above the threshold for complete melting throughout the film thickness, the liquid phase can be deeply undercooled before solidification. As a result, the vacancy diffusion in the resolidified region is limited and the region is trapped in the metastable chemically disordered state. Laser pulsing below the threshold forms a limited supercooled surface region that solidifies at sufficiently high temperatures, enabling diffusion-assisted reordering. This demonstrates that ultrafast lasers can achieve subtle atomic rearrangements in bimetallic alloys in a reversible and nonvolatile fashion.

Spatially resolved investigation of all optical magnetization switching in TbFe alloys.

Optical control of magnetization using femtosecond laser without applying any external magnetic field offers the advantage of switching magnetic states at ultrashort time scales. Recently, all-optical helicity-dependent switching (AO-HDS) has drawn a significant attention for potential information and data storage device applications. In this work, we employ element and magnetization sensitive photoemission electron microscopy (PEEM) to investigate the role of heating in AO-HDS for thin films of the rare-earth transition-metal alloy TbFe. Spatially resolved measurements in a 3-5 µm sized stationary laser spot demonstrate that AO-HDS is a local phenomenon in the vicinity of thermal demagnetization in a 'ring' shaped region. The efficiency of AO-HDS further depends on a local temperature profile around the demagnetized region and thermally activated domain wall motion. We also demonstrate that the thickness of the film determines the preferential switching direction for a particular helicity.

Imaging of buried 3D magnetic rolled-up nanomembranes.

Increasing performance and enabling novel functionalities of microelectronic devices, such as three-dimensional (3D) on-chip architectures in optics, electronics, and magnetics, calls for new approaches in both fabrication and characterization. Up to now, 3D magnetic architectures had mainly been studied by integral means without providing insight into local magnetic microstructures that determine the device performance. We prove a concept that allows for imaging magnetic domain patterns in buried 3D objects, for example, magnetic tubular architectures with multiple windings. The approach is based on utilizing the shadow contrast in transmission X-ray magnetic circular dichroism (XMCD) photoemission electron microscopy and correlating the observed 2D projection of the 3D magnetic domains with simulated XMCD patterns. That way, we are not only able to assess magnetic states but also monitor the field-driven evolution of the magnetic domain patterns in individual windings of buried magnetic rolled-up nanomembranes.

Strong interlayer coupling in van der Waals heterostructures built from single-layer chalcogenides.

Semiconductor heterostructures are the fundamental platform for many important device applications such as lasers, light-emitting diodes, solar cells, and high-electron-mobility transistors. Analogous to traditional heterostructures, layered transition metal dichalcogenide heterostructures can be designed and built by assembling individual single layers into functional multilayer structures, but in principle with atomically sharp interfaces, no interdiffusion of atoms, digitally controlled layered components, and no lattice parameter constraints. Nonetheless, the optoelectronic behavior of this new type of van der Waals (vdW) semiconductor heterostructure is unknown at the single-layer limit. Specifically, it is experimentally unknown whether the optical transitions will be spatially direct or indirect in such hetero-bilayers. Here, we investigate artificial semiconductor heterostructures built from single-layer WSe2 and MoS2. We observe a large Stokes-like shift of ∼ 100 meV between the photoluminescence peak and the lowest absorption peak that is consistent with a type II band alignment having spatially direct absorption but spatially indirect emission. Notably, the photoluminescence intensity of this spatially indirect transition is strong, suggesting strong interlayer coupling of charge carriers. This coupling at the hetero-interface can be readily tuned by inserting dielectric layers into the vdW gap, consisting of hexagonal BN. Consequently, the generic nature of this interlayer coupling provides a new degree of freedom in band engineering and is expected to yield a new family of semiconductor heterostructures having tunable optoelectronic properties with customized composite layers.

Printing nearly-discrete magnetic patterns using chemical disorder induced ferromagnetism.

Ferromagnetism in certain alloys consisting of magnetic and nonmagnetic species can be activated by the presence of chemical disorder. This phenomenon is linked to an increase in the number of nearest-neighbor magnetic atoms and local variations in the electronic band structure due to the existence of disorder sites. An approach to induce disorder is through exposure of the chemically ordered alloy to energetic ions; collision cascades formed by the ions knock atoms from their ordered sites and the concomitant vacancies are filled randomly via thermal diffusion of atoms at room temperature. The ordered structure thereby undergoes a transition into a metastable solid solution. Here we demonstrate the patterning of highly resolved magnetic structures by taking advantage of the large increase in the saturation magnetization of Fe60Al40 alloy triggered by subtle atomic displacements. The sigmoidal characteristic and sensitive dependence of the induced magnetization on the atomic displacements manifests a sub-50 nm patterning resolution. Patterning of magnetic regions in the form of stripes separated by ∼ 40 nm wide spacers was performed, wherein the magnet/spacer/magnet structure exhibits reprogrammable parallel (↑/spacer/↑) and antiparallel (↑/spacer/↓) magnetization configurations in zero field. Materials in which the magnetic behavior can be tuned via ion-induced phase transitions may allow the fabrication of novel spin-transport and memory devices using existing lateral patterning tools.

Magnetic dipole and higher pole interaction on a square lattice.

We have studied the magnetic interaction of circular magnetic islands with a dipole character on a square lattice. The square pattern consists of lithographically prepared polycrystalline PdFe islands, 150 nm in diameter and a periodicity of 300 nm. Below the Curie temperature at 260 K, the islands are in a single domain state with isotropic in-plane magnetization. Below 160 K, there is an onset of interisland interaction that leads to a change of the shape of the hysteresis, an increase of coercivity, and a development of in-plane anisotropy. Photoemission electron microscopy with circularly polarized incident x rays tuned to the L3 edge of Fe confirms the increasing correlation of the magnetic islands and the formation of elongated chains, as predicted by Vedmedenko et al. [Phys. Rev. Lett. 95, 207202 (2005)] for contributions from pole interactions of higher order than the dipolar one. Neighboring chains are found to be irregularly oriented either parallel or antiparallel.