Direct observation of twisted stacking domains in the van der Waals magnet CrI3.

Van der Waals (vdW) stacking is a powerful technique to achieve desired properties in condensed matter systems through layer-by-layer crystal engineering. A remarkable example is the control over the twist angle between artificially-stacked vdW crystals, enabling the realization of unconventional phenomena in moiré structures ranging from superconductivity to strongly correlated magnetism. Here, we report the appearance of unusual 120° twisted faults in vdW magnet CrI3 crystals. In exfoliated samples, we observe vertical twisted domains with a thickness below 10 nm. The size and distribution of twisted domains strongly depend on the sample preparation methods, with as-synthesized unexfoliated samples showing tenfold thicker domains than exfoliated samples. Cooling induces changes in the relative populations among different twisting domains, rather than the previously assumed structural phase transition to the rhombohedral stacking. The stacking disorder induced by sample fabrication processes may explain the unresolved thickness-dependent magnetic coupling observed in CrI3.

Understanding the Effect of Curvature on the Magnetization Reversal of Three-Dimensional Nanohelices.

Comprehending the interaction between geometry and magnetism in three-dimensional (3D) nanostructures is important to understand the fundamental physics of domain wall (DW) formation and pinning. Here, we use focused-electron-beam-induced deposition to fabricate magnetic nanohelices with increasing helical curvature with height. Using electron tomography and Lorentz transmission electron microscopy, we reconstruct the 3D structure and magnetization of the nanohelices. The surface curvature, helical curvature, and torsion of the nanohelices are then quantified from the tomographic reconstructions. Furthermore, by using the experimental 3D reconstructions as inputs for micromagnetic simulations, we can reveal the influence of surface and helical curvature on the magnetic reversal mechanism. Hence, we can directly correlate the magnetic behavior of a 3D nanohelix to its experimental structure. These results demonstrate how the control of geometry in nanohelices can be utilized in the stabilization of DWs and control of the response of the nanostructure to applied magnetic fields.

Topological Spin Textures in an Insulating van der Waals Ferromagnet.

Generation and control of topological spin textures constitutes one of the most exciting challenges of modern spintronics given their potential applications in information storage technologies. Of particular interest are magnetic insulators, which due to low damping, absence of Joule heating and reduced dissipation can provide energy-efficient spin-textures platform. Here, it is demonstrated that the interplay between sample thickness, external magnetic fields, and optical excitations can generate a prolific paramount of spin textures, and their coexistence in insulating CrBr3 van der Waals (vdW) ferromagnets. Using high-resolution magnetic force microscopy and large-scale micromagnetic simulation methods, the existence of a large region in T-B phase diagram is demonstrated where different stripe domains, skyrmion crystals, and magnetic domains exist and can be intrinsically selected or transformed to each-other via a phase-switch mechanism. Lorentz transmission electron microscopy unveils the mixed chirality of the magnetic textures that are of Bloch-type at given conditions but can be further manipulated into Néel-type or hybrid-type via thickness-engineering. The topological phase transformation between the different magnetic objects can be further inspected by standard photoluminescence optical probes resolved by circular polarization indicative of an existence of exciton-skyrmion coupling mechanism. The findings identify vdW magnetic insulators as a promising framework of materials for the manipulation and generation of highly ordered skyrmion lattices relevant for device integration at the atomic level.

Raman Shifts in Two-Dimensional van der Waals Magnets Reveal Magnetic Texture Evolution.

Two-dimensional (2D) van der Waals magnets comprise rich physics that can be exploited for spintronic applications. We investigate the interplay between spin-phonon coupling and spin textures in a 2D van der Waals magnet by combining magneto-Raman spectroscopy with cryogenic Lorentz transmission electron microscopy. We find that when stable skyrmion bubbles are formed in the 2D magnet, a field-dependent Raman shift can be observed, and this shift is absent for the 2D magnet prepared in its ferromagnetic state. Correlating these observations with numerical simulations that take into account field-dependent magnetic textures and spin--phonon coupling in the 2D magnet, we associate the Raman shift to field-induced modulations of the skyrmion bubbles and derive the existence of inhomogeneity in the skyrmion textures over the film thickness.

Thermal Hysteresis and Ordering Behavior of Magnetic Skyrmion Lattices.

The physics of phase transitions in two-dimensional (2D) systems underpins research in diverse fields including statistical mechanics, nanomagnetism, and soft condensed matter. However, many aspects of 2D phase transitions are still not well understood, including the effects of interparticle potential, polydispersity, and particle shape. Magnetic skyrmions are chiral spin-structure quasi-particles that form two-dimensional lattices. Here, we show, by real-space imaging using in situ cryo-Lorentz transmission electron microscopy coupled with machine learning image analysis, the ordering behavior of Néel skyrmion lattices in van der Waals Fe3GeTe2. We demonstrate a distinct change in the skyrmion size distribution during field-cooling, which leads to a loss of lattice order and an evolution of the skyrmion liquid phase. Remarkably, the lattice order is restored during field heating and demonstrates a thermal hysteresis. This behavior is explained by the skyrmion energy landscape and demonstrates the potential to control the lattice order in 2D phase transitions.

Orientational Disorder in Epitaxially Connected Quantum Dot Solids.

Periodic arrays of strongly coupled colloidal quantum dots (QDs) may enable unprecedented control of electronic band structure through manipulation of QD size, shape, composition, spacing, and assembly geometry. This includes the possibilities of precisely engineered bandgaps and charge carrier mobilities, as well as remarkable behaviors such as metal-insulator transitions, massless carriers, and topological states. However, experimental realization of these theoretically predicted electronic structures is presently limited by structural disorder. Here, we use aberration-corrected scanning transmission electron microscopy to precisely quantify the orientational disorder of epitaxially connected QD films. In spite of coherent atomic connectivity between nearest neighbor QDs, we find misalignment persists with a standard deviation of 1.9°, resulting in significant bending strain localized to the adjoining necks. We observe and quantify a range of out-of-plane particle orientations over thousands of QDs and correlate the in-plane and out-of-plane misalignments, finding QDs misoriented out-of-plane display a statistically greater misalignment with respect to their in-plane neighbors as well. Using the bond orientational order metric ψ4, we characterize the 4-fold symmetry and introduce a quantification of the local superlattice (SL) orientation. This enables direct comparison between local orientational order in the SL and atomic lattice (AL). We find significantly larger variations in the SL orientation and a statistically robust but locally highly variable correlation between the orientations of the two differently scaled lattices. Distinct AL and SL behaviors are observed about a grain boundary, with a sharp boundary in the AL orientations, but a more smooth transition in the SL, facilitated by lattice deformation between the neighboring grains. Coupling between the AL and SL is a fundamental driver of film growth, and these results suggest nontrivial underlying mechanics, implying that simplified models of epitaxial attachment may be insufficient to understand QD growth and disorder when oriented attachment and superlattice growth occur in concert.