The magnetic moment of rare earth elements originates from electrons in the partially filled 4f orbitals. Accessing this moment electrically by scanning tunneling spectroscopy is hampered by shielding of outer-lying orbitals. Here we show that we can detect the magnetic moment of an individual Ce atom adsorbed on a Cu2N ultrathin film on Cu(100) by using a sensor tip that has its apex functionalized with a Kondo screened spin system. We calibrate the sensor tip by deliberately coupling it to a well characterized Fe atom. Subsequently, we use the splitting of the tip's Kondo resonance when approaching a spectroscopically dark Ce atom to sense its magnetic moment.
The interactions between carbon nanotubes (CNTs) and metal adatoms as well as metal contacts are studied by means of ab initio electronic structure calculations. We show that the electronic properties of a semiconducting (8,4) CNT can be modified by small amounts of Pd adatoms. Such a decoration conserves the piezoelectric properties of the CNT. Besides the electronic influence, the stability of a single adatom, which is of big importance for future technology applications, is investigated as well. We find only small energy barriers for the diffusion of a Pd adatom on the CNT surface. Thus, si…
We propose a new universal mechanism that makes it possible to drive an individual atomic spin using a spin polarized scanning tunnel microscope (STM) with an oscillating electric signal. We show that the combination of the distance dependent exchange with the magnetic tip and the electrically driven mechanical oscillation of the surface spins permits to control their quantum state. Based on a combination of density functional theory and multiplet calculations, we show that the proposed mechanism is essential to account for the recently observed electrically driven paramagnetic spin resonance …
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…
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 magnet…
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)…
We demonstrate using inelastic scanning tunneling spectroscopy (ISTS) and simulations based on density functional theory that the amplitude and sign of the magnetic anisotropy energy for a single Fe atom adsorbed onto the Pt(111) surface can be manipulated by modifying the adatom binding site. Since the magnitude of the measured anisotropy is remarkably small, up to an order of magnitude smaller than previously reported, electron-hole excitations are weak and thus the spin-excitation exhibits long lived precessional lifetimes compared to the values found for the same adatom on noble metal surf…
We study magnetism of an adatom adsorbed on AA-stacked bilayer graphene (BLG) in both unbiased and biased cases, using the Anderson impurity model. We find different magnetic phase diagrams for the adatom, depending on the energy level of the adatom, which varies from the magnetic phase diagram of adatom in normal metals to that in graphene. This is due to the individual energy dependence of the density of states (DOS) of AA-stacked BLG and anomalous broadening of the adatom energy level. Furthermore we investigate the effect of a bias voltage on DOS of AA-stacked and show that the magnetizati…
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 …
A comprehensive theory is presented for the voltage, temperature, and spatial dependence of the tunneling current between a scanning tunneling microscope (STM) tip and a metallic surface with an individual magnetic adatom. Modeling the adatom by a nondegenerate Anderson impurity, a general expression is derived for a weak tunneling current in terms of the dressed impurity Green function, the impurity-free surface Green function, and the tunneling matrix elements. This generalizes Fano's analysis to the interacting case. The differential-conductance lineshapes seen in recent STM experiments wit…
Using density functional theory, we investigate the electronic and magnetic properties of $3d$ transition-metal adatoms adsorbed on a monolayer of Mn on W(110). Mn/W(110) has a noncollinear cycloidal spin-spiral ground state with an angle of 173$^\circ$ between magnetic moments of adjacent Mn rows. It allows to rotate the spin orientation of an adsorbed magnetic adatom quasi-continuously. Therefore, this surface is ideally suited for manipulating the spin direction of individual atoms and exploring their magnetic properties using scanning tunneling microscopy (STM). The adsorbed V and Cr trans…
Magnetic adatoms on surfaces are exchange coupled to their environment, inducing fast relaxation of excited spin states and decoherence. These interactions can be suppressed by inserting decoupling layers between the magnetic adsorbate and the metallic substrate. Using low-temperature scanning tunneling microscopy and spectroscopy, we investigate the magnetic properties of single Fe atoms on Au(111) covered by a monolayer of MoS$_2$ and explore the influence of the moiré structure on the spin excitation spectra. Fe adatoms absorbed at minima of the moiré structure exhibit almost pure inelastic…
The electronic and magnetic properties of individual Fe atoms adsorbed on the surface of the topological insulator Bi$_2$Te$_3$(111) are investigated. Scanning tunneling microscopy and spectroscopy prove the existence of two distinct types of Fe species, while our first-principles calculations assign them to Fe adatoms in the hcp and fcc hollow sites. The combination of x-ray magnetic circular dichroism measurements and angular dependent magnetization curves reveals out-of-plane anisotropies for both species with anisotropy constants of $K_{\text{fcc}} = (10 \pm 4)$ meV/atom and $K_{\text{hcp}…
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 …
An understanding of the pinning of magnetic skyrmions to defects is crucial for the development of future spintronic applications. While pinning is desirable for a precise positioning of magnetic skyrmions it is detrimental when they are to be moved through a material. We use scanning tunneling microscopy to study the interaction between atomic scale defects and magnetic skyrmions that are only a few nanometers in diameter. The studied pinning centers range from single atom inlayer defects and adatoms to clusters adsorbed on the surface of our model system. We find very different pinning stren…
CO-terminated tips currently provide the best spatial resolution obtainable in atomic force microscopy. Due to their chemical inertness, they allow to probe interactions dominated by Pauli repulsion. The small size and inertness of the oxygen front atom yields unprecedented resolution of organic molecules, metal clusters and surfaces. We study the capability of CO-terminated tips to laterally manipulate single iron adatoms on the Cu(111) surface with combined atomic force and scanning tunneling microscopy at 7\,K. Furthermore, we find that even a slight asymmetry of the tip results in a distor…
A combined experimental and theoretical study of doping individual Fe atoms into Bi2Se3 is presented. It is shown through a scanning tunneling microscopy study that single Fe atoms initially located at hollow sites on top of the surface (adatoms) can be incorporated into subsurface layers by thermally-activated diffusion. Angle-resolved photoemission spectroscopy in combination with ab-initio calculations suggest that the doping behavior changes from electron donation for the Fe adatom to neutral or electron acceptance for Fe incorporated into substitutional Bi sites. According to first princi…
We use Ca doping during growth of one and two monolayer thick MgO films on Ag(100) to identify the adsorption sites of individual adatoms with scanning tunneling microscopy. For this we combine atomic resolution images of the bare MgO layer with images of the adsorbates and the substitutional Ca atoms taken at larger tip-sample distance. For Ho atoms, the adsorption sites depend on MgO thickness. On the monolayer, they are distributed on the O and bridge sites according to the abundance of those sites, 1/3 and 2/3 respectively. On the MgO bilayer, Ho atoms populate almost exclusively the O sit…
Coherent control of individual atomic and molecular spins on surfaces has recently been demonstrated by using electron spin resonance (ESR) in a scanning tunneling microscope (STM). Here we present a combined experimental and modeling study of the ESR of a single hydrogenated Ti atom that is exchange-coupled to a Fe adatom located in 0.6-0.8 nm away. Continuous wave and pulsed ESR of the Ti spin showed a Rabi rate with two contributions, one from the tip and the other from the Fe, whose spin interactions with Ti were modulated by the radio-frequency electric field. The Fe contribution is compa…
We review the problem of spin decoherence of magnetic atoms deposited on a surface. Recent breakthroughs in scanning tunnelling microscopy (STM) make it possible to probe the spin dynamics of individual atoms, either isolated or integrated in nanoengineered spin structures. Transport pump and probe techniques with spin polarized tips permit measuring the spin relaxation time $T_1$, while novel demonstration of electrically driven STM single spin resonance has provided a direct measurement of the spin decoherence time $T_2$ of an individual magnetic adatom. Here we address the problem of spin d…
Rare-earth related electron spins in crystalline hosts are unique material systems, as they can potentially provide a direct interface between telecom band photons and long-lived spin quantum bits. Specifically, their optically accessible electron spins in solids interacting with nuclear spins in their environment are valuable quantum memory resources. Detection of nearby individual nuclear spins, so far exclusively shown for few dilute nuclear spin bath host systems such as the NV center in diamond or the silicon vacancy in silicon carbide, remained an open challenge for rare-earths in their …
We experimentally demonstrate the use of a single electronic spin to measure the quantum dynamics of distant individual nuclear spins from within a surrounding spin bath. Our technique exploits coherent control of the electron spin, allowing us to isolate and monitor nuclear spins weakly coupled to the electron spin. Specifically, we detect the evolution of distant individual carbon-13 nuclear spins coupled to single nitrogen vacancy centers in a diamond lattice with hyperfine couplings down to a factor of 8 below the electronic spin bare dephasing rate. Potential applications to nanoscale mag…
Individual, luminescent point defects in solids so called color centers are atomic-sized quantum systems enabling sensing and imaging with nanoscale spatial resolution. In this overview, we introduce nanoscale sensing based on individual nitrogen vacancy (NV) centers in diamond. We discuss two central challenges of the field: First, the creation of highly-coherent, shallow NV centers less than 10 nm below the surface of single-crystal diamond. Second, the fabrication of tip-like photonic nanostructures that enable efficient fluorescence collection and can be used for scanning probe imaging bas…
We demonstrate an all-optical method for magnetic sensing of individual molecules in ambient conditions at room temperature. Our approach is based on shallow nitrogen-vacancy (NV) centers near the surface of a diamond crystal, which we use to detect single paramagnetic molecules covalently attached to the diamond surface. The manipulation and readout of the NV centers is all-optical and provides a sensitive probe of the magnetic field fluctuations stemming from the dynamics of the electronic spins of the attached molecules. As a specific example, we demonstrate detection of a single paramagnet…
Electron spins in solids constitute remarkable quantum sensors. Individual defect centers in diamond were used to detect individual nuclear spins with nanometer scale resolution, and ensemble magnetometers rival SQUID and vapor cell magnetometers when taking into account room temperature operation and size. NV center spins can also detect electric field vectors, despite their weak coupling to electric fields. %even that of an isolated fundamental charge, despite their weak coupling to electric fields. Here, we employ ensembles of NV center spins to measure macroscopic AC electric vector fields…
Institut de Science et d’Ingénierie Supramoléculaires (ISIS, UMR7006), Université de Strasbourg（斯特拉斯堡大学超分子科学与工程学院）；Institut für Physik, Johannes Gutenberg Universität Mainz（美因茨约翰内斯·古腾堡大学物理研究所）；Department of Physics, Texas AM University（德克萨斯农工大学物理系）；Max Planck Institute for the Physics of Complex Systems（马克斯·普朗克复杂系统物理研究所）；Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；Institute of Physics, Czech Academy of Sciences（捷克科学院物理研究所）；Department of Physics, The State University of New York at Buffalo（纽约州立大学布法罗分校物理系）
