Spin-Glass States Generated in a van der Waals Magnet by Alkali-Ion Intercalation.

Tuning magnetic properties in layered van der Waals (vdW) materials has captured significant attention due to the efficient control of ground states by heterostructuring and external stimuli. Electron doping by electrostatic gating, interfacial charge transfer, and intercalation is particularly effective in manipulating the exchange and spin-orbit properties, resulting in a control of Curie temperature (TC) and magnetic anisotropy. Here, an uncharted role of intercalation is discovered to generate magnetic frustration. As a model study, Na atoms are intercalated into the vdW gaps of pristine Cr2Ge2Te6 (CGT) where generated magnetic frustration leads to emerging spin-glass states coexisting with a ferromagnetic order. A series of dynamic magnetic susceptibility measurements/analysis confirms the formation of magnetic clusters representing slow dynamics with a distribution of relaxation times. The intercalation also modifies other macroscopic physical parameters including the significant enhancement of TC from 66 to 240 K and the switching of magnetic easy-hard axis direction. This study identifies intercalation as a unique route to generate emerging frustrated spin states in simple vdW crystals.

Laser-induced topological spin switching in a 2D van der Waals magnet.

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. However, little is known about the interplay between light and spin properties in vdW layers. Here we show that ultrafast laser excitation can not only generate different type of spin textures in CrGeTe3 vdW magnets but also induce a reversible transformation between them in a topological toggle switch mechanism. Our atomistic spin dynamics simulations and wide-field Kerr microscopy measurements show that different textures can be generated via high-intense laser pulses within the picosecond regime. 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. Our results indicate laser-driven spin textures on 2D magnets as a pathway towards reconfigurable topological architectures at the atomistic level.

Probing spin dynamics of ultra-thin van der Waals magnets via photon-magnon coupling.

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 Cr2Ge2Te6 (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.

Tunable gigahertz dynamics of low-temperature skyrmion lattice in a chiral magnet.

Recently, it has been shown that the chiral magnetic insulator Cu2OSeO3hosts 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 Cu2OSeO3. LTSs are populated via a field cycling protocol with the static magnetic field applied parallel to the ⟨100⟩ crystalline direction of plate and cuboid-shaped bulk crystals. By analyzing temperature-dependent broadband spectroscopy data, clear evidence of LTS excitations with clockwise (CW), counterclockwise (CCW), and breathing mode (BR) character at temperatures belowT= 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 Cu2OSeO3crystals 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.