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The design and control of atomic-scale spin structures constitute major challenges for spin-based quantum technology platforms, including quantum dots, color centers, and molecular spins. Here, we showcase a strategy for designing the quantum properties of molecular spin qubits by combining tip-assisted on-surface assembly with electron spin resonance scanning tunneling microscopy (ESR-STM): We fabricate magnetic dimer complexes that consist of an iron phthalocyanine (FePc) molecule and an organometallic half-sandwich complex formed by the FePc ligand and an attached iron atom, Fe(C6H6). The total complex forms a mixed-spin (1/2,1) quantum ferrimagnet with a well-separated correlated ground state doublet, which we utilize for coherent control. As a result of the correlation, the quantum ferrimagnet shows an improved spin lifetime (>1.5 ${\mu}$s) as it is partially protected against inelastic electron scattering. Lastly, the ferrimagnet units also enable intermolecular coupling, that can be used to realize both ferromagnetic or antiferromagnetic structures. Thus, quantum ferrimagnets provide a versatile platform to improve coherent control in general and to study complex magnetic interactions., Comment: 17 pages, 4 figures

Nuclear spins owe their long-lived magnetic states to their excellent isolation from the environment. At the same time, a finite degree of interaction with their surroundings is necessary for reading and writing the spin state. Therefore, detailed knowledge of and control over the atomic environment of a nuclear spin is key to optimizing conditions for quantum information applications. While various platforms enabled single-shot readout of nuclear spins, their direct environments were either unknown or impossible to controllably modify on the atomic scale. Scanning tunnelling microscopy (STM), combined with electron spin resonance (ESR), provides atomic-scale information of individual nuclear spins via the hyperfine interaction. Here, we demonstrate single-shot readout of an individual $^{\text{49}}$Ti nuclear spin with an STM. Employing a pulsed measurement scheme, we find its lifetime to be in the order of seconds. Furthermore, we shed light on the pumping and relaxation mechanisms of the nuclear spin by investigating its response to both ESR driving and tunnelling current, which is supported by model calculations. These findings give an atomic-scale insight into the nature of nuclear spin relaxation and are relevant for the development of atomically assembled qubit platforms., Comment: 27 pages, 5 figures, 2 extended data figures, 3 supplementary sections, 6 supplementary figures, 1 supplementary table

The nuclear spin, being much more isolated from the environment than its electronic counterpart, enables quantum experiments with prolonged coherence times and presents a gateway towards uncovering the intricate dynamics within an atom. These qualities have been demonstrated in a variety of nuclear spin qubit architectures, albeit with limited control over the direct environment of the nuclei. As a contrasting approach, the combination of electron spin resonance (ESR) and scanning tunnelling microscopy (STM) provides a bottom-up platform to study the fundamental properties of nuclear spins of single atoms on a surface. However, access to the time evolution of these nuclear spins, as was recently demonstrated for electron spins, remained a challenge. Here, we present an experiment resolving the nanosecond coherent dynamics of a hyperfine-driven flip-flop interaction between the spin of an individual nucleus and that of an orbiting electron. We use the unique local controllability of the magnetic field emanating from the STM probe tip to bring the electron and nuclear spins in tune, as evidenced by a set of avoided level crossings in ESR-STM. Subsequently, we polarize both spins through scattering of tunnelling electrons and measure the resulting free evolution of the coupled spin system using a DC pump-probe scheme. The latter reveals a complex pattern of multiple interfering coherent oscillations, providing unique insight into the atom's hyperfine physics. The ability to trace the coherent hyperfine dynamics with atomic-scale structural control adds a new dimension to the study of on-surface spins, offering a pathway towards dynamic quantum simulation of low-dimensional magnonics.

Historically, electron spin resonance (ESR) has provided excellent insight into the electronic, magnetic, and chemical structure of samples hosting spin centers. In particular, the hyperfine interaction between the electron and the nuclear spins yields valuable structural information of these centers. In recent years, the combination of ESR and scanning tunneling microscopy (ESR-STM) has allowed to acquire such information on individual spin centers of magnetic atoms bound atop a surface, while additionally providing spatial information about the binding site. Here, we conduct a full angle-dependent investigation of the hyperfine splitting for individual titanium atoms on MgO/Ag(001) by measurements in a vector magnetic field. We observe strong anisotropy in both the g-factor and the hyperfine tensor. Combining the results of the hyperfine splitting with the symmetry properties of the binding site obtained from STM images and a basic point charge model allows us to predict the shape of the electronic ground state configuration of the titanium atom. Relying on experimental values only, this method paves the way for a new protocol for electronic structure analysis for spin centers on surfaces.

Spin resonance of single spin centers bears great potential for chemical structure analysis, quantum sensing and quantum coherent manipulation. Essential for these experiments is the presence of a two-level spin system whose energy splitting can be chosen by applying a magnetic field. In recent years, a combination of electron spin resonance (ESR) and scanning tunneling microscopy (STM) has been demonstrated as a technique to detect magnetic properties of single atoms on surfaces and to achieve sub-${\mu}$eV energy resolution. Nevertheless, up to now the role of the required magnetic fields has not been elucidated. Here, we perform single-atom ESR on individual Fe atoms adsorbed on magnesium oxide (MgO), using a 2D vector magnetic field as well as the local field of the magnetic STM tip in a commercially available STM. We show how the ESR amplitude can be greatly improved by optimizing the magnetic fields, revealing in particular an enhanced signal at large in-plane magnetic fields. Moreover, we demonstrate that the stray field from the magnetic STM tip is a versatile tool. We use it here to drive the electron spin more efficiently and to perform ESR measurements at constant frequency by employing tip-field sweeps. Lastly, we show that it is possible to perform ESR using only the tip field, under zero external magnetic field, which promises to make this technique available in many existing STM systems.

Graphene, the first true two-dimensional material still reveals the most remarkable transport properties among the growing class of two-dimensional materials. Although many studies have investigated fundamental scattering processes, the surprisingly large variation in the experimentally determined resistances associated with a localized defect is still an open issue. Here, we quantitatively investigate the local transport properties of graphene prepared by polymer assisted sublimation growth (PASG) using scanning tunneling potentiometry. PASG graphene is characterized by a spatially homogeneous current density, which allows to analyze variations in the local electrochemical potential with high precision. We utilize this possibility by examining the local sheet resistance finding a significant variation of up to 270% at low temperatures. We identify a correlation of the sheet resistance with the stacking sequence of the 6H-SiC substrate as well as with the distance between the graphene sheet and the substrate. Our results experimentally quantify the strong impact of the graphene-substrate interaction on the local transport properties of graphene., Comment: 27 pages main text, 4 figures and 11 pages supplementary information, 17 figures. This is a pre-print of an article published in Nature Communications

Shrinking spintronic devices to the nanoscale ultimately requires localized control of individual atomic magnetic moments. At these length scales, the exchange interaction plays important roles, such as in the stabilization of spin-quantization axes, the production of spin frustration, and creation of magnetic ordering. Here, we demonstrate the precise control of the exchange bias experienced by a single atom on a surface, covering an energy range of four orders of magnitude. The exchange interaction is continuously tunable from milli-eV to micro-eV by adjusting the separation between a spin-1/2 atom on a surface and the magnetic tip of a scanning tunneling microscope (STM). We seamlessly combine inelastic electron tunneling spectroscopy (IETS) and electron spin resonance (ESR) to map out the different energy scales. This control of exchange bias over a wide span of energies provides versatile control of spin states, with applications ranging from precise tuning of quantum state properties, to strong exchange bias for local spin doping. In addition we show that a time-varying exchange interaction generates a localized AC magnetic field that resonantly drives the surface spin. The static and dynamic control of the exchange interaction at the atomic-scale provides a new tool to tune the quantum states of coupled-spin systems.

Magnetic resonance imaging (MRI) revolutionized diagnostic medicine and biomedical research by allowing a noninvasive access to spin ensembles. To enhance MRI resolution to the nanometer scale, new approaches including scanning probe methods have been used in recent years, which culminated in detection of individual spins. This allowed three-dimensional (3D) visualization of organic samples and of sophisticated spin-structures. Here, we demonstrate for the first time MRI of individual atoms on a surface. The setup, implemented in a cryogenic scanning tunneling microscope (STM), uses single-atom electron spin resonance (ESR) to achieve sub-{\AA}ngstr\"om resolution exceeding the spatial resolution of previous experiments by one to two orders of magnitude. We find that MRI scans of different atomic species and probe tips lead to unique signatures in the resonance images. These signatures reveal the magnetic interactions between the tip and the atom, in particular magnetic dipolar and exchange interaction.

Manipulation of spin states at the single-atom scale underlies spin-based quantum information processing and spintronic devices. Such applications require protection of the spin states against quantum decoherence due to interactions with the environment. While a single spin is easily disrupted, a coupled-spin system can resist decoherence by employing a subspace of states that is immune to magnetic field fluctuations. Here, we engineered the magnetic interactions between the electron spins of two spin-1/2 atoms to create a clock transition and thus enhance their spin coherence. To construct and electrically access the desired spin structures, we use atom manipulation combined with electron spin resonance (ESR) in a scanning tunneling microscope (STM). We show that a two-level system composed of a singlet state and a triplet state is insensitive to local and global magnetic field noise, resulting in much longer spin coherence times compared with individual atoms. Moreover, the spin decoherence resulting from the interaction with tunneling electrons is markedly reduced by a homodyne readout of ESR. These results demonstrate that atomically-precise spin structures can be designed and assembled to yield enhanced quantum coherence.

Quantum spin networks having engineered geometries and interactions are eagerly pursued for quantum simulation and access to emergent quantum phenomena such as spin liquids. Spin-1/2 centers are particularly desirable because they readily manifest coherent quantum fluctuations. Here we introduce a controllable spin-1/2 architecture consisting of titanium atoms on a magnesium oxide surface. We tailor the spin interactions by atomic-precision positioning using a scanning tunneling microscope (STM), and subsequently perform electron spin resonance (ESR) on individual atoms to drive transitions into and out of quantum eigenstates of the coupled-spin system. Interactions between the atoms are mapped over a range of distances extending from highly anisotropic dipole coupling, to strong exchange coupling. The local magnetic field of the magnetic STM tip serves to precisely tune the superposition states of a pair of spins. The precise control of the spin-spin interactions and ability to probe the states of the coupled-spin network by addressing individual spins will enable exploration of quantum many-body systems based on networks of spin-1/2 atoms on surfaces.

The highest-density magnetic storage media will code data in single-atom bits. To date, the smallest individually addressable bistable magnetic bits on surfaces consist of 5-12 atoms. Long magnetic relaxation times were demonstrated in molecular magnets containing one lanthanide atom, and recently in ensembles of single holmium (Ho) atoms supported on magnesium oxide (MgO). Those experiments indicated the possibility for data storage at the fundamental limit, but it remained unclear how to access the individual magnetic centers. Here we demonstrate the reading and writing of individual Ho atoms on MgO, and show that they independently retain their magnetic information over many hours. We read the Ho states by tunnel magnetoresistance and write with current pulses using a scanning tunneling microscope. The magnetic origin of the long-lived states is confirmed by single-atom electron paramagnetic resonance (EPR) on a nearby Fe sensor atom, which shows that Ho has a large out-of-plane moment of $(10.1 \pm 0.1)$ $\mu_{\rm B}$ on this surface. In order to demonstrate independent reading and writing, we built an atomic scale structure with two Ho bits to which we write the four possible states and which we read out remotely by EPR. The high magnetic stability combined with electrical reading and writing shows that single-atom magnetic memory is possible.