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Combining electron paramagnetic resonance (EPR) with scanning tunneling microscopy (STM) enables detailed insight into the interactions and magnetic properties of single atoms on surfaces. A requirement for EPR-STM is the efficient coupling of microwave excitations to the tunnel junction. Here, we achieve a coupling efficiency of the order of unity by using a radiofrequency antenna placed parallel to the STM tip, which we interpret using a simple capacitive-coupling model. We further demonstrate the possibility to perform EPR-STM routinely above 4 K using amplitude as well as frequency modulation of the radiofrequency excitation. We directly compare different acquisition modes on hydrogenated Ti atoms and highlight the advantages of frequency and magnetic field sweeps as well as amplitude and frequency modulation in order to maximize the EPR signal. The possibility to tune the microwave-excitation scheme and to perform EPR-STM at relatively high temperature and high power opens this technique to a broad range of experiments, ranging from pulsed EPR spectroscopy to coherent spin manipulation of single atom ensembles., Comment: 17 pages, 7 figures

We report on the magnetic properties of Fe and Co adatoms on a Cu$_{2}$N/Cu(100)-$c(2 \times 2)$ surface investigated by x-ray magnetic dichroism measurements and density functional theory (DFT) calculations including the local coulomb interaction. We compare these results with properties formerly deduced from STM spin excitation spectroscopy (SES) performed on the individual adatoms. In particular we focus on the values of the local magnetic moments determined by XMCD compared to the expectation values derived from the description of the SES data.The angular dependence of the projected magnetic moments along the magnetic field, as measured by XMCD, can be understood on the basis of the SES Hamiltonian. In agreement with DFT, the XMCD measurements show large orbital contributions to the total magnetic moment for both magnetic adatoms.

We combine density functional theory, x-ray magnetic circular dichroism, multiplet calculations, and scanning tunneling spectroscopy to assess the magnetic properties of Fe atoms adsorbed on a thin layer of MgO(100) on Ag(100). Despite the strong axial field due to the O ligand, the weak cubic field induced by the four-fold coordination to Mg atoms entirely quenches the first order orbital moment. This is in marked contrast to Co, which has an out-of-plane orbital moment of $L_z = \pm 3$ that is protected from mixing in a cubic ligand field. The spin-orbit interaction restores a large fraction of the Fe orbital moment leading a zero-field splitting of $14.0 \pm 0.3$~meV, the largest value reported for surface adsorbed Fe atoms., Comment: 6 pages, 4 figures

The robustness of the gapless topological surface state hosted by a 3D topological insulator against perturbations of magnetic origin has been the focus of recent investigations. We present a comprehensive study of the magnetic properties of Fe impurities on a prototypical 3D topological insulator Bi$_2$Se$_3$ using local low temperature scanning tunneling microscopy and integral x-ray magnetic circular dichroism techniques. Single Fe adatoms on the Bi$_2$Se$_3$ surface, in the coverage range $\approx 1%$ are heavily relaxed into the surface and exhibit a magnetic easy axis within the surface-plane, contrary to what was assumed in recent investigations on the opening of a gap. Using \textit{ab initio} approaches, we demonstrate that an in-plane easy axis arises from the combination of the crystal field and dynamic hybridization effects., Comment: 5 pages, 3 figures, typos corrected