The orbital magnetic moment is still surprisingly not well understood, in contrast to the spin part. Its description in finite systems, such as isolated atoms and molecules, is not problematic, but it was only recently that a rigorous picture was provided for extended systems. Here we focus on an intermediate class of systems: magnetic adatoms placed on a non-magnetic surface. We show that the essential quantity is the ground-state charge current density, in the presence of spin-orbit coupling, and set out its first-principles description. This is illustrated by studying the magnetism of the surface Pt electrons, induced by the presence of Cr, Mn, Fe, Co and Ni adatoms. A physically appealing partition of the charge current is introduced. This reveals that there is an important nonlocal contribution to the orbital moments of the Pt atoms, extending three times as far from each magnetic adatom as the induced spin and local orbital moments. We find that it is as sizable as the latter, and attribute its origin to a spin-orbital susceptibility of the Pt surface, different from the one responsible for the formation of the local orbital moments.
We have performed density functional theory calculations of graphene decorated with carbon adatoms, which bind at the bridge site of a C--C bond. Earlier studies have shown that the C adatoms have magnetic moments and have suggested the possibility of ferromagnetism with high Curie temperature. Here we propose to use a gate voltage to fine tune the magnetic moments from zero to 1$μ_B$ while changing the magnetic coupling from antiferromagnetism to ferromagnetism and again to antiferromagnetism. These results are rationalized within the Stoner and RKKY models. When the SCAN meta-GGA correction …
We present a first-principles study of the surface magnetism induced by Cr, Mn, Fe and Co adatoms on the (111) surfaces of Rh, Pd, Ag, Ir, Pt and Au. We first describe how the different contributions to the surface magnetism enter the magnetic stray field, with special attention paid to the induced orbital moments. Then we present results for the spin and orbital magnetic moments of the adatoms, and for the induced surface spin and orbital magnetic moments, the latter being further divided into atomic and inter-atomic contributions. We investigate how the surface magnetism is determined by the…
Hydrogen adatoms induced magnetic moment on graphene has been observed in atomic scale in a recent experiment [Gonzalez-Herrero et al., Science 352, 437 (2016)]. Here, we demonstrate that all the experimental phenomena can be simply and well described by an equivalent Anderson impurity model, where the electronic correlations on both carbon and hydrogen atoms are represented by an effective on-site Coulomb interaction on hydrogen adatom $U_H$. This simple equivalent model works so well is because that the main effect of Coulomb interaction on both carbon and hydrogen atoms is just to split the…
Single adatoms offer an exceptional playground for studying magnetism and its associated dynamics at the atomic scale. Here we review recent results on single adatoms deposited on metallic substrates, based on time-dependent density functional theory. First we analyze quantum zero-point spin-fluctuations (ZPSF) as calculated from the fluctuation-dissipation theorem, and show how they affect the magnetic stability by modifying the magnetic anisotropy energy. We also assess the impact of ZPSF in the limit of small hybridization to the substrate characteristic of semi-insulating substrates, conne…
The phase diagram of graphene decorated with magnetic adatoms distributed either on a single sublattice, or evenly over the two sublattices, is computed for adatom concentrations as low as $\sim1\%$. Within the framework of the $s$-$d$ interaction, we take into account disorder effects due to the random positioning of the adatoms and/or to the thermal fluctuations in the direction of magnetic moments. Despite the presence of disorder, the magnetic phases are shown to be stable down to the lowest concentration accessed here. This result agrees with several experimental observations where adatom…
Individual nuclear spin states can have very long lifetimes and could be useful as qubits. Progress in this direction was achieved on MgO/Ag(001) via detection of the hyperfine interaction (HFI) of Fe, Ti and Cu adatoms using scanning tunneling microscopy (STM). Previously, we systematically quantified from first-principles the HFI for the whole series of 3d transition adatoms (Sc-Cu) deposited on various ultra-thin insulators, establishing the trends of the computed HFI with respect to the filling of the magnetic s- and d-orbitals of the adatoms and on the bonding with the substrate. Here we …
The creation of magnetism on non-magnetic semiconductor surfaces is of importance for the realization of spintronics devices. Especially, the coupling of electron spins within quantum nanostructures can be utilized for nanomagnetism applications. Here, we demonstrate, based on first-principles density-functional theory calculations, that the adsorption of H atoms on the Si(111)-(7$\times$7) surface induces the spin polarization of surrounding Si dangling bonds (DBs) and their spin orderings. It is revealed that the H adsorption on a rest-atom site exhibits a Jahn-Teller-like distortion that ac…
RKKY-like contributions to the magnetic anisotropy energy: 3d adatoms on Pt(111) surface
磁各向异性能定义了稳定磁矩的能垒。利用密度泛函理论为基础的模拟和分析配方，我们建立，这个障碍是强烈修改的长程贡献非常类似的Frieden振荡和Rudermann-Kittel-Kasuya-Yosida相互作用。因此，预期并观察到振荡，具有不同的衰减因子和在现实材料中的高度各向异性，其可以非平凡地切换磁各向异性能量的符号。这种行为是普遍的，为了说明，我们解决了过渡金属吸附原子，Cr，Mn，Fe和Co沉积在Pt（111）表面。我们特别解释了导致Fe吸附原子在Pt（111）表面上观察到的磁各向异性能的强位置依赖性的机制，如先前通过基于第一性原理的模拟和非弹性扫描隧道光谱所揭示的那样（A. A. Khajetoorians等人，Phys. Rev. Lett. 111，157204（2013））。对于Pd或Rh（111）表面上的Fe吸附原子和Rh（111）表面上的Co吸附原子获得的磁各向异性能的位置依赖性，相同的机制可能是有效的（P. Blonski et al.Phys.Rev.B81，104426（2010））。
We show that an individual adatom on a magnetic surface can exhibit a noncollinear spin density. Using density functional theory we study Co and Ir adatoms on a Mn monolayer on the W(110) surface which possesses a noncollinear canted spin structure. Due to hybridization with the nearest and next-nearest Mn atoms of the monolayer the spin direction of the underlying substrate is encoded into the orbitals of the adatom. This explains recent scanning tunneling microscopy experiments showing a spin sensitive shape asymmetry of adatoms [Serrate \emph{et al.}, Phys. Rev. B \textbf{93}, 125424 (2016)…
Nuclear spins are among the potential candidates prospected for quantum information technology. A recent breakthrough enabled to atomically resolve their interaction with the electron spin, the so-called hyperfine interaction, within individual atoms utilizing scanning tunneling microscopy (STM). Intriguingly, this was only realized for a few species put on a two-layers thick MgO. Here, we systematically quantify from first-principles the hyperfine interactions of the whole series of 3d transition adatoms deposited on various thicknesses of MgO, NaF, NaCl, h--BN and Cu$_2$N films. We identify …
We propose a reversible mechanism for switching Heisenberg-type exchange interactions between deposited transition metal adatoms from ferromagnetic to antiferromagnetic. Using first-principles calculations, we show that this mechanism can be realized for cobalt atoms on the surface of black phosphorus by making use of electrically-controlled orbital repopulation, as recently demonstrated by scanning probe techniques [Nat. Commun. 9, 3904 (2018)]. We find that field-induced repopulation not only affects the spin state, but also causes considerable modification of exchange interaction between ad…
Low-temperature scanning tunneling microscopy is used here to study dynamic bonding of gold atoms on surfaces under low coordination conditions. In the experiments, using an atomically-sharp gold tip, a gold adatom is deposited onto a gold surface with atomic precision either on the first hollow site near a step edge, or far away from it. Classical molecular dynamics simulations at 4.2 K and density functional theory calculations serve to elucidate the difference in the bonding behavior between these two different placements, while also providing information on the crystalline classification o…
We report scanning tunneling microscopy studies of individual adatoms deposited on an InSb(110) surface. The adatoms can be reproducibly dropped off from the STM tip by voltage pulses, and impact tunneling into the surface by up to ~100x. The spatial extent and magnitude of the tunneling effect are widely tunable by imaging conditions such as bias voltage, set current and photoillumination. We attribute the effect to occupation of a (+/0) charge transition level, and switching of the associated adatom-induced band bending. The effect in STM topographic images is well reproduced by transport mo…
Theoretical and experimental investigation of the electronic and magnetic structure of transition metal atoms on an insulating interface with a metallic substrate at low temperatures is quite challenging. In this paper, we show a density functional theory plus Hubbard $U$ based protocol to study an Mn adatom on three symmetrically allowed absorption sites, namely on O, hollow (between two Mg and two O) and on Mg on MgO(001). We added a thick enough(bulk-like) metallic Ag slab beneath MgO for faithful replication of scanning tunneling microscopy (STM) experiments. Our study reveals that to dete…
Chains of magnetic adatoms on superconductors have been discussed as promising systems for realizing Majorana end states. Here, we show that dilute Yu-Shiba-Rusinov (YSR) chains are also a versatile platform for quantum magnetism and correlated electron dynamics, with widely adjustable spin values and couplings. Focusing on subgap excitations, we derive an extended $t-J$ model for dilute quantum YSR chains and use it to study the phase diagram as well as tunneling spectra. We explore the implications of quantum magnetism for the formation of a topological superconducting phase, contrasting it …
Lanthanide atoms and molecules are promising candidates for atomic data storage and quantum logic due to the long magnetic lifetime of their electron quantum states. Accessing these states through electrical transport requires the engineering of their electronic configuration down to the level of individual atomic orbitals. Here, we address the magnetism of surface-supported lanthanide atoms, clusters, and films with orbital selectivity using X-ray absorption spectroscopy and magnetic circular dichroism. We exploit the selection rules of electric dipole transitions to reveal the occupation and…
Inducing a robust long-range magnetic order in diamagnetic graphene remains a challenge. While nitrogen-doped graphene is reported to be a promising candidate, the corresponding exchange mechanism endures unclear and is essential to tune further and manipulate magnetism. Within the first-principles calculations, we systematically investigate the local moment formation and the concurrent interaction between various defect complexes. The importance of adatom diffusion on the differential defect abundance is discussed. The individual nitrogen complexes that contribute toward itinerant and a local…
Supercurrent detection and manipulation of topological phase transitions in Shiba-Majorana hybrid systems
Physical Research Laboratory（物理研究实验室）；Technische Universität Braunschweig（布伦瑞克工业大学）；The Hamburg Centre for Ultrafast Imaging（汉堡超快成像中心）；Universität Hamburg（汉堡大学）；International Research Centre MagTop, Institute of Physics, Polish Academy of Sciences（波兰科学院物理研究所磁拓扑国际研究中心）；University of Basel（巴塞尔大学）
Despite extensive experimental and theoretical efforts, the important issue of the effects of surface magnetic impurities on the topological surface state of a topological insulator (TI) remains unresolved. We elucidate the effects of Cr impurities on epitaxial thin films of (Bi$_{0.5}$Sb$_{0.5}$)$_{2}$Te$_{3}$: Cr adatoms are incrementally deposited onto the TI held in ultrahigh vacuum at low temperatures, and \textit{in situ} magnetoconductivity and Hall effect measurements are performed at each increment with electrostatic gating. In the experimentally identified surface transport regime, t…
Tailoring magnetism of nanographenes via tip-controlled dehydrogenation
Empa—Swiss Federal Laboratories for Materials Science and Technology（瑞士联邦材料科技研究院）；Technical University of Dresden（德累斯顿工业大学）；University of Zurich（苏黎世大学）；University of Bern（伯尔尼大学）；Max Planck Institute of Microstructure Physics（马克斯·普朗克微观结构物理研究所）
We observe an unusual behavior of the spin Hall magnetoresistance (SMR) measured in a Pt ultra-thin film deposited on a ferromagnetic insulator, which is a tensile-strained LaCoO3 (LCO) thin film with the Curie temperature Tc=85K. The SMR displays a strong magnetic-field dependence below Tc, with the SMR amplitude continuing to increase (linearly) with increasing the field far beyond the saturation value of the ferromagnet. The SMR amplitude decreases gradually with raising the temperature across Tc and remains measurable even above Tc. Moreover, no hysteresis is observed in the field dependen…
Motivated by recent experiments, here we study the indirect interactions between magnetic impurities deposited on top of a clean Pb(110) surface induced by the underlying conduction electrons. Our approach makes use of \textit{ab initio} calculations to characterize the clean Pb(110) surface and avoids self-consistency, a feature that greatly reduces the computational cost. In combination with 2$^{\text{nd}}$ order perturbation theory in the microscopic \textit{s-d} exchange parameter $J_{K}$ between a magnetic adatom and the conduction electrons, we are able to systematically derive the Ruder…
