2023, Yang, Wei, Rosenkranz, Marco, Velkos, Georgios, Ziegs, Frank, Dubrovin, Vasilii, Schiemenz, Sandra, Spree, Lukas, de Souza Barbosa, Matheus Felipe, Guillemard, Charles, Valvidares, Manuel, Büchner, Bernd, Liu, Fupin, Avdoshenko, Stanislav M., Popov, Alexey A.

Nd-based nitride clusterfullerenes NdM2N@C80 with rare-earth metals of different sizes (M = Sc, Y, Lu) were synthesized to elucidate the influence of the cluster composition, shape and internal strain on the structural and magnetic properties. Single crystal X-ray diffraction revealed a very short Nd-N bond length in NdSc2N@C80. For Lu and Y analogs, the further shortening of the Nd-N bond and pyramidalization of the NdM2N cluster are predicted by DFT calculations as a result of the increased cluster size and a strain caused by the limited size of the fullerene cage. The short distance between Nd and nitride ions leads to a very large ligand-field splitting of Nd3+ of 1100-1200 cm−1, while the variation of the NdM2N cluster composition and concomitant internal strain results in the noticeable modulation of the splitting, which could be directly assessed from the well-resolved fine structure in the Nd-based photoluminescence spectra of NdM2N@C80 clusterfullerenes. Photoluminescence measurements also revealed an unprecedentedly strong nephelauxetic effect, pointing to a high degree of covalency. The latter appears detrimental to the magnetic axiality despite the strong ligand field. As a result, the ground magnetic state has considerable transversal components of the pseudospin g-tensor, and the slow magnetic relaxation of NdSc2N@C80 could be observed by AC magnetometry only in the presence of a magnetic field. A combination of the well-resolved magneto-optical states and slow relaxation of magnetization suggests that Nd clusterfullerenes can be useful building blocks for magneto-photonic quantum technologies.

2021, Lopes, J. Marcelo J., Czubak, Dietmar, Zallo, Eugenio, Figueroa, Adriana I., Guillemard, Charles, Valvidares, Manuel, Rubio-Zuazo, Juan, López-Sanchéz, Jesús, Valenzuela, Sergio O., Hanke, Michael, Ramsteiner, Manfred

Scalable fabrication of magnetic 2D materials and heterostructures constitutes a crucial step for scaling down current spintronic devices and the development of novel spintronic applications. Here, we report on van der Waals (vdW) epitaxy of the layered magnetic metal Fe3GeTe2 (FGT) - a 2D crystal with highly tunable properties and a high prospect for room temperature ferromagnetism (FM) - directly on graphene by employing molecular beam epitaxy. Morphological and structural characterization confirmed the realization of large-area, continuous FGT/graphene heterostructure films with stable interfaces and good crystalline quality. Furthermore, magneto-transport and x-ray magnetic circular dichroism investigations confirmed a robust out-of-plane FM in the layers, comparable to state-of-the-art exfoliated flakes from bulk crystals. These results are highly relevant for further research on wafer-scale growth of vdW heterostructures combining FGT with other layered crystals such as transition metal dichalcogenides for the realization of multifunctional, atomically thin devices. © 2021 The Author(s).