The ability to efficiently control topological magnetism is crucial for advancing technological applications and deepening our understanding of magnetic systems. Although emerging van der Waals (vdW) multiferroics present a promising frontier for energy-efficient spin manipulation, the control of topological magnetism remains challenging due to its scarcity in multiferroics. Here, we demonstrate that highly tunable merons and antimerons emerge in monolayer multiferroic CuCrP₂S₆ (CCPS). The antiferroelectric-to-ferroelectric (AFE-FE) transition enhances exchange couplings, notably reducing meron density and increasing meron size during cooling. Merons exhibit unique dynamics, characterized by nontrivial attraction and annihilation processes, which generates distinct long-lived spin waves and reduces meron number difference between AFE and FE phases until they vanish. Importantly, ultrafast laser pulses can induce ferroelectricity-tunable merons from a uniform in-plane magnetization, re-leading to a large difference in meron density between the AFE and FE phases. These findings enhance our understanding of topological magnetism and open up exciting avenues for controlling the properties and dynamics of topological states through electrical and optical methods.

Despite extensive research on magnetic skyrmions and antiskyrmions, a significant challenge remains in crafting nontrivial high-order skyrmionic textures with varying, or even tailor-made, topologies. We address this challenge, by focusing on a construction pathway of skyrmionic metamaterials within a monolayer thin film and suggest several skyrmionic metamaterials that are surprisingly stable, i.e., long-lived, due to a self-stabilization mechanism. This makes these new textures promising for applications. Central to our approach is the concept of ’simulated controlled assembly’, in short, a protocol inspired by ’click chemistry’ that allows for positioning topological magnetic structures where one likes, and then allowing for energy minimization to elucidate the stability. Utilizing high-throughput atomistic-spin-dynamic simulations alongside state-of-the-art AI-driven tools, we have isolated skyrmions (topological charge Q = 1), antiskyrmions (Q = − 1), and skyrmionium (Q = 0). These entities serve as foundational ’skyrmionic building blocks’ to form the here-reported intricate textures. In this work, two key contributions are introduced to the field of skyrmionic systems. First, we present a novel combination of atomistic spin dynamics simulations and controlled assembly protocols for the stabilization and investigation of new topological magnets. Second, using the aforementioned methods we report on the discovery of skyrmionic metamaterials.

Among the quasi-two-dimensional van der Waals magnetic systems, Fe4⁢Ge⁢Te2 makes a profound impact due to its near-room-temperature ferromagnetic behavior and the complex magnetothermal phase diagram exhibiting multiple phase transformations, as observed from magnetization and magnetotransport measurements. A complete analysis of these phase transformations in light of electronic correlation and its impact on the underlying magnetic interactions remain unexplored in the existing literature. Using first-principles methodologies, incorporating the dynamical nature of electron correlation, we have analyzed the interplay of the direction of magnetization in an easy-plane and easy-axis manner with the underlying crystal symmetry, which reveals the opening of a pseudogap feature beyond the spin-reorientation transition temperature. The impact of dynamical correlation on the calculated magnetic circular dichroism and x-ray absorption spectrum of the 𝐿-edge of Fe atoms compare well with existing experimental observations. The calculated intersite Heisenberg exchange interactions display a complicated nature, depending upon the pairwise interactions among the two inequivalent Fe sites, indicating a Ruderman-Kittel-Kasuya-Yosida-like behavior of the magnetic interactions. We note the existence of significant anisotropic and antisymmetric exchange interactions, resulting in a chirality in the magnetic behavior of the system. Subsequent investigation of the dynamical aspects of magnetism in Fe4⁢Ge⁢Te2 and the respective magnetothermal phase diagram reveals that the dynamical nature of spins and the decoupling of the magnetic properties for both sites of Fe is crucial to explain all the experimentally observed phase transformations. 

Non-trivial band topology along with magnetism leads to different novel quantum phases. When time-reversal symmetry is broken in three-dimensional topological insulators (TIs) through, e.g., the proximity effect, different phases such as the quantum Hall phase or the quantum anomalous Hall(QAH) phase emerge, displaying interesting transport properties for spintronic applications. The QAH phase displays sidewall chiral edge states, which leads to the QAH effect. We have considered a heterostructure consisting of a TI, namely Bi[Formula: see text]Se[Formula: see text], sandwiched between two two-dimensional ferromagnetic monolayers of CrI[Formula: see text], to study how its topological and transport properties change due to the proximity effect. Combining DFT and tight-binding calculations, along with non-equilibrium Green's function formalism, we show that a well-defined exchange gap appears in the band structure in which spin-polarised edge states flow. In a finite slab, the nature of the surface states depends on both the cross-section and thickness of the system. Therefore, we also study the width and finite-size effects on the transmission and topological properties of this magnetised TI nanoribbon.

PdFe/Ir(111) has attracted tremendous attention for next-generation spintronics devices due to existence of magnetic skyrmions with the external magnetic field. Our density functional theoretical calculations in combination with spin dynamics simulation suggest that the spin spiral phase in fcc stacked PdFe/Ir(111) flips into the skyrmion lattice phase around B-ert similar to 6 T. This leads to the microscopic understanding of the thermodynamic and kinetic behaviours affected by the intrinsic spin-lattice couplings (SLCs) in this skyrmion material for magneto-mechanical properties. Here we calculate fully relativistic SLC parameters from first principle computations and investigate the effect of SLC on dynamical magnetic interactions in skyrmion multilayers PdFe/Ir(111). The exchange interactions arising from next nearest-neighbors (NN) in this material are highly frustrated and responsible for enhancing skyrmion stability. We report the larger spin-lattice effect on both dynamical Heisenberg exchanges and Dzyaloshinskii-Moriya interactions for next NN compared to NN which is in contrast with recently observed spin-lattice effect in bulk bcc Fe and CrI3 monolayer. Based on our analysis, we find that the effective measures of SLCs in fcc (hcp) stacking of PdFe/Ir(111) are similar to 2.71(similar to 2.36) and similar to 14.71(similar to 21.89) times stronger for NN and next NN respectively, compared to bcc Fe. The linear regime of displacement for SLC parameters is <= 0.02 angstrom which is 0.72% of the lattice constant for PdFe/Ir(111). The microscopic understanding of SLCs provided by our current study could help in designing spintronic devices based on thermodynamic properties of skyrmion multilayers.

Magnetoelasticity plays a crucial role in numerous magnetic phenomena, including magnetocalorics, magnon excitation via acoustic waves, and ultrafast demagnetization, or the Einstein-de Haas effect. Despite a long-standing discussion on anisotropy-mediated magnetoelastic interactions of relativistic origin, the exchange-mediated magnetoelastic parameters within an atomistic framework have only recently begun to be investigated. As a result, many of their behaviors and values for real materials remain poorly understood. Therefore, by using a proposed simple modification of the embedded cluster approach that reduces the computational complexity, we critically analyze the properties of exchange-mediated spin-lattice coupling parameters for elemental 3d ferromagnets (bcc Fe, fcc Ni, and fcc Co), comparing methods used for their extraction and relating their realistic values to symmetry considerations and orbitally decomposed contributions. Additionally, we investigate the effects of noncollinearity (spin temperature) and applied pressure on these parameters. For Fe, we find that single-site rotations, associated with spin temperatures around 100 K, induce significant modifications, particularly in Dzyaloshinskii-Moriya-type couplings; in contrast, such interactions in Co and Ni remain almost configuration independent. Moreover, we demonstrate a notable change in the exchange-mediated magnetoelastic constants for Fe under isotropic contraction. Finally, the conversion between atomistic, quantum-mechanically derived parameters and the phenomenological magnetoelastic theory is discussed, which can be a useful tool towards larger and more realistic dynamics simulations involving coupled subsystems.

Details on anisotropic magnon dispersion in van der Waals (vdW) ferromagnetic insulators CrPS4 and CrSBr are reported, driven by anisotropic Heisenberg exchange couplings arising from in-plane broken crystal symmetry. The anisotropic magnon dispersion contributes to longitudinal and transverse magnon currents generating the anisotropic spin Seebeck effect (ASSE) and the thermal Hall effect (THE) accompanied with spin Nernst effect (SNE), requiring neither external magnetic field nor Berry curvature. In CrPS4, the ASSE exhibits a very large anisotropy ratio of over 100% as the thermal gradient along different main axes, and this ratio can be further tuned by temperature or a gate current. The THE and SNE unconstrained by spin-orbit coupling (SOC) emerge when the thermal gradient is not parallel to the main axis, characterized by a large Hall angle approximate to 0.4. Compared to CrPS4, CrSBr exhibits a more limited anisotropic magnon transport owing to the less variation in magnon group velocities along different main axes. Moreover, the reversed magnitude relationship of magnon group velocities leads to the transverse magnon current being oriented in the opposite direction. These findings identify low-symmetry vdW magnetic materials as a promising framework for generation and manipulation of anisotropic magnon transport, relevant for spincaloritronic devices in the ultrathin regime.

The impact of the local chemical environment on the Gilbert damping in the binary alloy Fe100-xCox is investigated, using computations based on density functional theory. By varying the alloy composition x as well as Fe-Co atom positions we reveal that the effective damping of the alloy is highly sensitive to the nearest-neighbor environment, especially to the amount of Co and the average distance between Co-Co atoms at nearest-neighbor sites. Both lead to a significant local increase (up to an order of magnitude) of the effective Gilbert damping, originating mainly from variations of the density of states at the Fermi energy. In a global perspective (i.e., making a configuration average for a real material), those differences in damping are masked by statistical averages. When low-temperature explicit atomistic dynamics simulations are performed, the impact of short-range disorder on local dynamics is observed to also alter the overall relaxation rate. Our results illustrate the possibility of local chemical engineering of the Gilbert damping, which may stimulate the study of new ways to tune and control materials aiming for spintronics applications.

Despite decades of research, the role of the lattice and its coupling to the magnetisation during ultrafast demagnetisation processes is still not fully understood. Here we report on studies of both explicit and implicit lattice effects on laser induced ultrafast demagnetisation of bcc Fe and fcc Co. We do this using atomistic spin- and lattice dynamics simulations following a heat-conserving three-temperature model. We show that this type of Langevin-based simulation is able to reproduce observed trends of the ultrafast magnetization dynamics of fcc Co and bcc Fe. The parameters used in our models are all obtained from electronic structure theory, with the exception of the lattice dynamics damping term, where a range of parameters were investigated. It was found that while the explicit spin-lattice coupling in the studied systems does not impact the demagnetisation process notably, the lattice damping has a large influence on the details of the magnetization dynamics. The dynamics of Fe and Co following the absorption of a femtosecond laser pulse are compared with previous results for Ni and similarities and differences in the materials’ behavior are analysed. For all elements investigated so far with this model, we obtain a linear relationship between the value of the maximally demagnetized state and the fluence of the laser pulse, which is in agreement with experiments. Moreover, we demonstrate that the demagnetization amplitude is largest for Ni and smallest for Co. This holds over a wide range of the reported electron-phonon couplings, and this demagnetization trend is in agreement with recent experiments.

We developed a method which performs the coupled adiabatic spin and lattice dynamics based on the tight-binding electronic structure model, where the intrinsic magnetic field and ionic forces are calculated from the converged self-consistent electronic structure at every time step. By doing so, this method allows us to explore limits where the physics described by a parameterized spin-lattice Hamiltonian is no longer accurate. We demonstrate how the lattice dynamics is strongly influenced by the underlying magnetic configuration, where disorder is able to induce significant lattice distortions. The presented method requires significantly less computational resources than ab initio methods, such as time-dependent density functional theory (TD-DFT). Compared to parameterized Hamiltonian-based methods, it also describes more accurately the dynamics of the coupled spin and lattice degrees of freedom, which becomes important outside of the regime of small lattice and spin fluctuations.