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Two-dimensional (2D) van der Waals (vdW) magnets represent one of the most promising horizons for energy-efficient spintronic applications because their broad range of electronic, magnetic and topological properties. Of particular interest is the control of the magnetic properties of 2D materials by femtosecond laser pulses which can provide a real path for low-power consumption device platforms in data storage industries. However, little is known about the interplay between light and spin properties in vdW layers. Here, combining large-scale spin dynamics simulations including biquadratic exchange interactions and wide-field Kerr microscopy (WFKM), we show that ultrafast laser excitation can not only generate different type of spin textures in CrGeTe$_3$ vdW magnets but also induce a reversible transformation between them in a toggle-switch mechanism. Our calculations show that skyrmions, anti-skyrmions, skyrmioniums and stripe domains can be generated via high-intense laser pulses within the picosecond regime. The effect is tunable with the laser energy where different spin behaviours can be selected, such as fast demagnetisation process ($\sim$250 fs) important for information technologies. The phase transformation between the different topological spin textures is obtained as additional laser pulses are applied to the system where the polarisation and final state of the spins can be controlled by external magnetic fields. We experimentally confirmed the creation, manipulation and toggle switching phenomena in CrGeTe$_3$ due to the unique aspect of laser-induced heating of electrons. Our results indicate laser-driven spin textures on 2D magnets as a pathway towards ultrafast reconfigurable architecture at the atomistic level.

Layered van der Waals (vdW) magnets can maintain a magnetic order even down to the single-layer regime and hold promise for integrated spintronic devices. While the magnetic ground state of vdW magnets was extensively studied, key parameters of spin dynamics, like the Gilbert damping, crucial for designing ultra-fast spintronic devices, remains largely unexplored. Despite recent studies by optical excitation and detection, achieving spin wave control with microwaves is highly desirable, as modern integrated information technologies predominantly are operated with these. The intrinsically small numbers of spins, however, poses a major challenge to this. Here, we present a hybrid approach to detect spin dynamics mediated by photon-magnon coupling between high-Q superconducting resonators and ultra-thin flakes of Cr$_2$Ge$_2$Te$_6$ (CGT) as thin as 11\,nm. We test and benchmark our technique with 23 individual CGT flakes and extract an upper limit for the Gilbert damping parameter. These results are crucial in designing on-chip integrated circuits using vdW magnets and offer prospects for probing spin dynamics of monolayer vdW magnets.

Recently, it has been shown that the chiral magnetic insulator Cu$_2$OSeO$_3$ hosts skyrmions in two separated pockets in temperature and magnetic field phase space. It has also been shown that the predominant stabilization mechanism for the low-temperature skyrmion (LTS) phase is via the crystalline anisotropy, opposed to temperature fluctuations that stabilize the well-established high-temperature skyrmion (HTS) phase. Here, we report on a detailed study of LTS generation by field cycling, probed by GHz spin dynamics in Cu$_2$OSeO$_3$. LTSs are populated via a field cycling protocol with the static magnetic field applied parallel to the $\langle{100}\rangle$ crystalline direction of plate and cuboid-shaped bulk crystals. By analyzing temperature-dependent broadband spectroscopy data, clear evidence of low-temperature skyrmion excitations with clockwise (CW), counterclockwise (CCW), and breathing mode (BR) character at temperatures below $T$ = 40 K are shown. We find that the mode intensities can be tuned with the number of field-cycles below the saturation field. By tracking the resonance frequencies, we are able to map out the field-cycle-generated LTS phase diagram, from which we conclude that the LTS phase is distinctly separated from the high-temperature counterpart. We also study the mode hybridization between the dark CW and the BR modes as a function of temperature. By using two Cu$_2$OSeO$_3$ crystals with different shapes and therefore different demagnetization factors, together with numerical calculations, we unambiguously show that the magnetocrystalline anisotropy plays a central role for the mode hybridization., Comment: 29 pages; main text: pages 1-29 with 7 figures, supplementary materials: pages 23-29 with 3 figures

The discovery of an ever increasing family of atomic layered magnetic materials, together with the already established vast catalogue of strong spin-orbit coupling (SOC) and topological systems, calls for some guiding principles to tailor and optimize novel spin transport and optical properties at their interfaces. Here we focus on the latest developments in both fields that have brought them closer together and make them ripe for future fruitful synergy. After outlining fundamentals on van der Waals (vdW) magnetism and SOC effects, we discuss how their coexistence, manipulation and competition could ultimately establish new ways to engineer robust spin textures and drive the generation and dynamics of spin current and magnetization switching in 2D materials-based vdW heterostructures. Grounding our analysis on existing experimental results and theoretical considerations, we draw a prospective analysis about how intertwined magnetism and spin-orbit torque (SOT) phenomena combine at interfaces with well-defined symmetries, and how this dictates the nature and figures-of-merit of SOT and angular momentum transfer. This will serve as a guiding role in designing future non-volatile memory devices that utilize the unique properties of 2D materials with the spin degree of freedom., Comment: 26 pages, 5 figures, 1 table and 1 textbox

Topologically protected nanoscale spin textures, known as magnetic skyrmions, possess particle-like properties and feature emergent magnetism effects. In bulk cubic heli-magnets, distinct skyrmion resonant modes are already identified using a technique like ferromagnetic resonance in spintronics. However, direct light-matter coupling between microwave photons and skyrmion resonance modes has not been demonstrated yet. Utilising two distinct cavity systems, we realise to observe a direct interaction between the cavity resonant mode and two resonant skyrmion modes, the counter-clockwise gyration and breathing modes, in bulk Cu$_2$OSeO$_3$. For both resonant modes, we find the largest coupling strength at 57 K indicated by an enhancement of the cavity linewidth at the degeneracy point. We study the effective coupling strength as a function of temperature within the expected skyrmion phase. We attribute the maximum in effective coupling strength to the presence of a large number of skyrmions, and correspondingly to a completely stable skyrmion lattice. Our experimental findings indicate that the coupling between photons and resonant modes of magnetic skyrmions depends on the relative density of these topological particles instead of the pure spin number in the system., Comment: 11 pages, main text: page 1-8 with 4 figures, supplementary material: page 9-11 with 6 figures

Electrical control of magnetism of a ferromagnetic semiconductor offers exciting prospects for future spintronic devices for processing and storing information. Here, we report observation of electrically modulated magnetic phase transition and magnetic anisotropy in thin crystal of Cr$_2$Ge$_2$Te$_6$ (CGT), a layered ferromagnetic semiconductor. We show that heavily electron-doped ($\sim$ $10^{14}$ cm$^{-2}$) CGT in an electric double-layer transistor device is found to exhibit hysteresis in magnetoresistance (MR), a clear signature of ferromagnetism, at temperatures up to above 200 K, which is significantly higher than the known Curie temperature of 61 K for an undoped material. Additionally, angle-dependent MR measurements reveal that the magnetic easy axis of this new ground state lies within the layer plane in stark contrast to the case of undoped CGT, whose easy axis points in the out-of-plane direction. We propose that significant doping promotes double-exchange mechanism mediated by free carriers, prevailing over the superexchange mechanism in the insulating state. Our findings highlight that electrostatic gating of this class of materials allows not only charge flow switching but also magnetic phase switching, evidencing their potential for spintronics applications.