Magnetic molecules are potential functional units for molecular and supramolecular spintronic devices. However, their magnetic and electronic properties depend critically on their interaction with metallic electrodes. Charge transfer and hybridization modify the electronic structure and thereby influence or even quench the molecular magnetic moment. Yet, detection and manipulation of the molecular spin state by means of charge transport, that is, spintronic functionality, mandates a certain level of hybridization of the magnetic orbitals with electrode states. Here we show how a judicious choice of the molecular spin centres determines these critical molecule–electrode contact characteristics. In contrast to late lanthanide analogues, the 4f-orbitals of single bis(phthalocyaninato)-neodymium(III) molecules adsorbed on Cu(100) can be directly accessed by scanning tunnelling microscopy. Hence, they contribute to charge transport, whereas their magnetic moment is sustained as evident from comparing spectroscopic data with ab initio calculations. Our results showcase how tailoring molecular orbitals can yield all-electrically controlled spintronic device concepts.

The unique properties of synchrotron radiation, such as broad energy spectrum, variable light polarization, and flexible time structure, have made it an enormously powerful tool in the study of magnetic phenomena and materials. The refinement of experimental techniques has led to many new research opportunities, keeping up with the challenges put up by modern magnetism research. In this contribution, we review some of the recent developments in the application of synchrotron radiation and particularly soft X-rays to current problems in magnetism, and we discuss future perspectives.

The interplay between chirality and magnetism is a source of fascination among scientists for over a century. In recent years, chirality‐induced spin selectivity (CISS) has attracted renewed interest. It is observed that electron transport through layers of homochiral molecules leads to a significant spin polarization of several tens of percent. Despite the abundant experimental evidence gathered through mesoscopic transport measurements, the exact mechanism behind CISS remains elusive. This study reports spin‐selective electron transport through single helical aromatic hydrocarbons that are sublimed in vacuo onto ferromagnetic cobalt surfaces and examined with spin‐polarized scanning tunneling microscopy (SP‐STM) at a temperature of 5 K. Direct comparison of two enantiomers under otherwise identical conditions revealed magnetochiral conductance asymmetries of up to 50% when either the molecular handedness is exchanged or the magnetization direction of the STM tip or Co substrate is reversed. Importantly, the results rule out electron–phonon coupling and ensemble effects as primary mechanisms responsible for CISS.

We have performed a combined spectroscopy and microscopy study on surfaces of ${\text{Sb}}_2{\text{Te}}_3/\text{Si}(111)$ thin films exposed to air and annealed under ultra-high vacuum conditions. Scanning tunneling microscopy images, with atomic resolution present in most areas of such processed surfaces, show a significant amount of impurities and defects. Scanning tunneling spectroscopy reveals the bulk band gap of $\sim 170\hspace{0.17em}\text{meV}$ centered $\sim 65\hspace{0.17em}\text{meV}$ above the Fermi level. This intrinsic p-type doping behavior is confirmed by high-resolution angle-resolved photoemission spectra, which show the dispersions of the lower Dirac cone and the spectral weight of the bulk valence bands crossing the Fermi level. Spin-polarized photoemission revealed up to ∼15% in-plane spin polarization for photoelectrons related to the topologically protected Dirac cone states near the Fermi level, and up to ∼40% for several states at higher binding energies. The results are interpreted using ab initio electronic structure simulations and confirm the robustness of the time-reversal symmetry protected topological surface states in ${\text{Sb}}_2{\text{Te}}_3$ in the presence of impurities and defects.

Electronic correlations play an important role in determining the properties of solid state systems, in particular, in the presence of narrow bands. In intermetallic alloys the strength of correlation effects and, thus, the details of the electronic structure depend on the concentration of the constituents, their interactions, and the degree of chemical order. Although the electronic structure of such a system can be conveniently studied by photoelectron spectroscopy, the interpretation of the spectra is nontrivial. To enable a quantitative analysis of chemically disordered systems showing correlation effects in photoemission spectroscopy we therefore incorporate dynamical mean-field theory in the fully relativistic version of layer-Korringa-Kohn-Rostoker theory and treat the results within the relativistic one-step model of photoemission generalized to the magnetic alloy case. Our ansatz allows the study of complex layered structures like thin films and multilayers and an almost naturally incorporation of a realistic surface barrier potential. We apply our theory to photoemission data of the magnetic alloy system ${\text{Ni}}_x{\text{Pd}}_{1-x}\left(001\right)$ and demonstrating that state-of-the-art photoemission theory is required to deal with this complex system. The comparison over a large alloy concentration range provides us with a means to disentangle the influence of alloying and correlation effects.

From the beginning of molecular theory, the interplay of chirality and magnetism has intrigued scientists. There is still the question if enantiospecific adsorption of chiral molecules occurs on magnetic surfaces. Enantiomer discrimination was conjectured to arise from chirality‐induced spin separation within the molecules and exchange interaction with the substrate's magnetization. Here, it is shown that single helical aromatic hydrocarbons undergo enantioselective adsorption on ferromagnetic cobalt surfaces. Spin and chirality sensitive scanning tunneling microscopy reveals that molecules of opposite handedness prefer adsorption onto cobalt islands with opposite out‐of‐plane magnetization. As mobility ceases in the final chemisorbed state, it is concluded that enantioselection must occur in a physisorbed transient precursor state. State‐of‐the‐art spin‐resolved ab initio simulations support this scenario by refuting enantio‐dependent chemisorption energies. These findings demonstrate that van der Waals interaction should also include spin‐fluctuations which are crucial for molecular magnetochiral processes.