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Magnetic impurities create in-gap states on superconductors. Recent experiments explore the topological properties of one-dimensional arrays of magnetic impurities on superconductors, because in certain regimes p-wave pairing can be locally induced leading to new topological phases. A byproduct of the new accessible phases is the appearance of zero-energy edge states that have non-Abelian exchange properties and can be used for topological quantum computation. Despite the large amount of theory devoted to these systems, most treatments use approximations that render their applicability limited when comparing with usual experiments of 1D impurity arrays on wide-band superconductors. These approximations either involve tight-binding-like approximations where the impurity energy scales match the minute energy scale of the superconducting gap and are many times unrealistic, or they assume strongly-bound in-gap states. Here, we use a theory for s-wave superconductors based on a wide-band normal metal, with any possible energy scale for the magnetic impurities and develop an efficient way of computing the well-known topological invariants of infinite chains. We perform concrete calculations on ferromagnetic spin chains using BCS Green's function for the superconductor and including Rashba coupling to compare with recent experimental results. The infinite-chain properties can be analytically obtained, giving us a way to compare with finite-chain calculations. We show that it is possible to converge to the infinite limit by doing finite-size numerical calculation, paving the way for numerical calculations not based on analytical Green's functions. As an application, we show that energy oscillations around zero with increasing number of atoms in the spin chain does not reflect the topological origin of the low-energy state., Financial support from the Spanish MICINN (Projects RTI2018-097895-B-C44 and Excelencia EUR2020-112116) and Eusko Jaurlaritza (Project PIBA_2020_1_0017) is gratefully acknowledged.

Electronic states in the gap of a superconductor inherit intriguing many-body properties from the superconductor. Here, we create these in-gap states by manipulating Cr atomic chains on the $\ensuremath{\beta}\ensuremath{-}\mathrm{Bi}{}_{2}\mathrm{Pd}$ superconductor. We find that the topological properties of the in-gap states can greatly vary depending on the crafted spin chain. These systems make an ideal platform for nontrivial topological phases because of the large atom-superconductor interactions and the existence of a large Rashba coupling at the Bi-terminated surface. We study two spin chains, one with atoms two lattice parameters apart and one with $\sqrt{2}$ lattice parameters. Of these, only the second one is in a topologically nontrivial phase, in agreement with the spin interactions for this geometry.

Combining the complex ordering ability of molecules with their local magnetic properties is a little-explored technique to tailor spin structures on surfaces. However, revealing the molecular geometry can be demanding. Nickelocene (Nc) molecules present a large spin-flip excitation leading to clear changes of conductance at the excitation-threshold bias. Using a superconducting tip, we have the energy resolution to detect small shifts of the Nc spin-flip excitation thresholds, permitting us to reveal the different individual environments of Nc molecules in an ordered layer. This knowledge allows us to reveal the adsorption configuration of a complex molecular structure formed by Nc molecules in different orientations and positions. As a consequence, we infer that Nc layers present a strong noncollinear magnetic-moment arrangement., Financial support from the Spanish MICINN (project RTI2018-097895-B-C44), the European H2020 FET open project MeMo (grant no. 766864), and the French Agence Nationale de la Recherche (grants no. ANR-13-BS10-0016, ANR-11-LABX-0058 NIE and ANR-10-LABX-0026 CSC) is gratefully acknowledged.

We investigated spin-1/2 hydrogenated titanium (Ti) atoms on MgO using scanning tunneling microscopy (STM) combined with electron spin resonance (ESR) in vector magnetic fields. Rotating external magnetic fields, we observed rather drastic changes in both amplitude and frequency of resonance signals for single Ti atoms. While the variation of ESR amplitudes reflects the effects of the spin polarization of a magnetic tip and local magnetic fields created by the interaction between the tip and Ti, the change of resonance frequencies shows the anisotropy of g values for Ti atoms. Using the Ti atoms at the low-symmetry bridge adsorption site of the MgO lattice allowed for identifying the g values in all three spatial directions. Multiplet calculations confirmed the origin of this anisotropy as the spin-orbit coupling induced effects of crystal. Our results show the capability of single atomic spins as a sensor to probe magnetic surroundings and highlight the precision of ESR-STM to identify the single atom's spin states in a solid-state environment., This work was supported by the Institute for Basic Science (Grant No. IBS-R027-D1). D.-J.C. acknowledges financial support from the Spanish MICINN (Project No. RTI2018- 097895-B-C44 and Excelencia Project No. EUR2020-112116) and Eusko Jaurlaritza (Project No. PIBA_2020_-1_0017). F.D. acknowledges financial support from Spanish MICINN (Grant No. PID2019-109539GB-C41), Basque Government (Grant No. IT986-16), and Canary Islands program Viera y Clavijo (Grant No. 2017/0000231). C.P.L. acknowledges financial support from the ONR.

The electrical control and readout of molecular spin states are key for high-density storage. Expectations are that electrically-driven spin and vibrational excitations in a molecule should give rise to new conductance features in the presence of magnetic anisotropy, offering alternative routes to study and, ultimately, manipulate molecular magnetism. Here, we use inelastic electron tunneling spectroscopy to promote and detect the excited spin states of a prototypical molecule with magnetic anisotropy. We demonstrate the existence of a vibron-assisted spin excitation that can exceed in energy and in amplitude a simple excitation among spin states. This excitation, which can be quenched by structural changes in the magnetic molecule, is explained using first-principles calculations that include dynamical electronic correlations., This work was supported by the Agence Nationale de la Recherche (grants No. ANR-13-BS10-0016, ANR-11-LABX-0058 NIE and ANR-10-LABX-0026 CSC) and by the Agencia Española de Investigación (grants Nos. MAT2016-78293-C6-1-R and MDM-2016-0618). D.-J.C. and N.L. thank the MICINN (project RTI2018-097895-B-C44). M.-L.B. thanks the national computational center CINES and TGCC (GENCI project: A0030807364).

Eigenstate multifractality is a distinctive feature of noninteracting disordered metals close to a metal-insulator transition, whose properties are expected to extend to superconductivity. While multifractality in three dimensions (3D) only develops near the critical point for specific strong-disorder strengths, multifractality in 2D systems is expected to be observable even for weak disorder. Here we provide evidence for multifractal features in the superconducting state of an intrinsic, weakly disordered single-layer NbSe2 by means of low-temperature scanning tunneling microscopy/spectroscopy. The superconducting gap, characterized by its width, depth, and coherence peaks' amplitude, shows a characteristic spatial modulation coincident with the periodicity of the quasiparticle interference pattern. The strong spatial inhomogeneity of the superconducting gap width, proportional to the local order parameter in the weak-disorder regime, follows a log-normal statistical distribution as well as a power-law decay of the two-point correlation function, in agreement with our theoretical model. Furthermore, the experimental singularity spectrum f(α) shows anomalous scaling behavior typical from 2D weakly disordered systems., We acknowledge financial support from AEI/FEDER-EU through the Maria de Maeztu unit of excellence MDM-2016-0618. This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under Contract No. DE-AC02-05CH11231. A.M.G.-G. acknowledges additional support from a Shanghai talent program and from the National Natural Science Foundation of China (NSFC) (Grant number 11874259).

Bulk and single-layer 2H-NbSe2 exhibit identical charge density wave order (CDW) with a quasi-commensurate 3 × 3 superlattice periodicity. Here we combine scanning tunnelling microscopy (STM) imaging at T = 1 K of 2H-NbSe2 with first-principles density functional theory (DFT) calculations to investigate the structural atomic rearrangement of this CDW phase. Our calculations for single-layers reveal that six different atomic structures are compatible with the 3 × 3 CDW distortion, although all of them lie on a very narrow energy range of at most 3 meV per formula unit, suggesting the coexistence of such structures. Our atomically resolved STM images of bulk 2H-NbSe2 unambiguously confirm this by identifying two of these structures. Remarkably, these structures differ from the X-ray crystal structure reported for the bulk 3 × 3 CDW which in fact is also one of the six DFT structures located for the single-layer. Our calculations also show that due to the minute energy difference between the different phases, the ground state of the 3 × 3 CDW could be extremely sensitive to doping, external strain or internal pressure within the crystal. The presence of multiphase CDW order in 2H-NbSe2 may provide further understanding of its low temperature state and the competition between different instabilities., Work at Bellaterra was supported by Spanish MINECO (Grants FIS2015-64886-C5-3-P and FIS2015-64886-C5-4-P, and the Severo Ochoa Centers of Excellence Program under Grants SEV-2017-0706 and SEV-2015-0496), Generalitat de Catalunya (Grant 2017SGR1506 and the CERCA Program) and by the European Union MaX Center of Excellence (Grant 824143). The work by B.G. has been performed in the context of the Physics Ph.D. program of the Universitat Autònoma de Barcelona. M.M.U acknowledges support by the Spanish MINECO under grant no. MAT2017-82074-ERC and by the ERC Starting grant “LINKSPM” (Grant 758558).

Bulk and single-layer 2 H-NbSe

Turning graphene magnetic is a promising challenge to make it an active material for spintronics. Predictions state that graphene structures with specific shapes can spontaneously develop magnetism driven by Coulomb repulsion of π-electrons, but its experimental verification is demanding. Here, we report on the observation and manipulation of individual magnetic moments in graphene open-shell nanostructures on a gold surface. Using scanning tunneling spectroscopy, we detect the presence of single electron spins localized around certain zigzag sites of the carbon backbone via the Kondo effect. We find near-by spins coupled into a singlet ground state and quantify their exchange interaction via singlet-triplet inelastic electron excitations. Theoretical simulations picture how electron correlations result in spin-polarized radical states with the experimentally observed spatial distributions. Extra hydrogen atoms bound to radical sites quench their magnetic moment and switch the spin of the nanostructure in half-integer amounts. Our work demonstrates the intrinsic π-paramagnetism of graphene nanostructures., π-magnetism in graphene systems has been predicted but remains an experimental challenge. Here the authors report the discovery of unpaired electron spins localized in certain sites of graphene nanoribbons, and the measurement of their coupling by inducing singlet-triplet excitations with a scanning tunneling microscope.

Magnetism at low dimensions is a thriving field of research with exciting opportunities in technology. This Colloquium focuses on the properties of 1D magnetic systems on solid surfaces. From the emulation of 1D quantum phases to the potential realization of Majorana edge states, spin chains are unique systems to study. The advent of scanning tunneling microscope (STM) based techniques has permitted us to engineer spin chains in an atom-by-atom fashion via atom manipulation and to access their spin states on the ultimate atomic scale. Here the current state of research on spin correlations and dynamics of atomic spin chains as studied by the STM is presented. After a brief review of the main properties of spin chains on solid surfaces, spin chains are classified according to the coupling of their magnetic moments with the holding substrate. This classification scheme takes into account that the nature and lifetimes of the spin-chain excitations intrinsically depend on the holding substrate. Interest is shown of using insulating layers on metals, which generally results in an increase in the spin state’s lifetimes such that their quantized nature gets evident and they are individually accessible. Next shown is the use of semiconductor substrates promising additional control through the tunable electron density via doping. When the coupling to the substrate is increased for spin chains on metals, the substrate conduction electron mediated interactions can lead to emergent exotic phases of the coupled spin chain-substrate conduction electron system. A particularly interesting example is furnished by superconductors. Magnetic impurities induce states in the superconducting gap. Because of the extended nature of the spin chain, the in-gap states develop into bands that can lead to the emergence of 1D topological superconductivity and consequently to the appearance of Majorana edge states. Finally, an outlook is given on the use of spin chains in spintronics, quantum communication, quantum computing, quantum simulations, and quantum sensors, D.-J. C. and N. L. acknowledge financial support from MICINN (RTI2018-097895-B-C44) and FEDER funds. J. W. and K. v. B. received funding from the Deutsche Forschungsgemeinschaft (DFG, German Research foundation)—SFB668. A. F. O. acknowledges support from the Netherlands Organisation for Scientific Research (NWO) and the European Research Council (ERC Starting Grant No. 676895 “SPINCAD”). A. J. H acknowledges support from the Institute for Basic Science under IBS-R027-D1

We thank Javier Zaldivar and Joeri de Bruijckere for developing the deconvolution process and Sebastian Bergeret for discussions. D.-J. C. and J. I. P. thank the European Union for support under the H2020-MSCA-IF-2014 Marie-Curie Individual Fellowship program (Proposal No. 654469), Spanish MINECO (MAT2016-78293-C6-1-R), Diputacion Foral de Gipuzkoa for Grant No. 64/15, and the European Regional Development Fund (ERDF). N. L. thanks Spanish MINECO (Grant No. MAT2015-66888-C3-2-R). M. M. U. acknowledges Spanish MINECO (MAT2014-60996-R). E. H., I. G., and H. S. acknowledge FIS2014-54498-R and MDM-2014-0377, COST MP16218 nanocohybri, ERC PNICTEYES Grant Agreement No. 679080, and Departamento Administrativo de Ciencia, Tecnologia e Innovacion, COLCIENCIAS (Colombia), Programa doctorados en el exterior and convocatoria 568-2012, as well as Comunidad de Madrid through program Nanofrontmag-CM (Grant No. S2013/MIT-2850)

We show that the magnetic ordering of coupled atomic dimers on a superconductor is revealed by their intragap spectral features. Chromium atoms on the superconductor β-Bi_{2}Pd surface display Yu-Shiba-Rusinov bound states, detected as pairs of intragap excitations in tunneling spectra. By means of atomic manipulation with a scanning tunneling microscope's tip, we form Cr dimers with different arrangements and find that their intragap features appear either shifted or split with respect to single atoms. These spectral variations are associated with the magnetic coupling, ferromagnetic or antiferromagnetic, of the dimer, as confirmed by density functional theory simulations. The striking qualitative differences between the observed tunneling spectra prove that intragap Shiba states are extremely sensitive to the magnetic ordering on the atomic scale.

Mixing of discretized states in quantum magnets has a radical impact on their properties. Managing this effect is key for spintronics in the quantum limit. Magnetic fields can modify state mixing and, for example, mitigate destabilizing effects in single-molecule magnets. The exchange bias field has been proposed as a mechanism for localized control of individual nanomagnets. Here, we demonstrate that exchange coupling with the magnetic tip of a scanning tunnelling microscope provides continuous tuning of spin state mixing in an individual nanomagnet. By directly measuring spin relaxation time with electronic pump-probe spectroscopy, we find that the exchange interaction acts analogously to a local magnetic field that can be applied to a specific atom. It can be tuned in strength by up to several tesla and cancel external magnetic fields, thereby demonstrating the feasibility of complete control over individual quantum magnets with atomically localized exchange coupling.

The creation of molecule-like structures in which magnetic atoms interact controllably is full of potential for the study of complex or strongly correlated systems. Here, we create spin chains in which a strongly correlated Kondo state emerges from magnetic coupling of transition-metal atoms. We build chains up to ten atoms in length by placing Fe and Mn atoms on a CuN surface with a scanning tunneling microscope. The atoms couple antiferromagnetically via superexchange interaction through the nitrogen atom network of the surface. The emergent Kondo resonance is spatially distributed along the chain. Its strength can be controlled by mixing atoms of different transition metal elements and manipulating their spatial distribution. We show that the Kondo screening of the full chain by the electrons of the nonmagnetic substrate depends on the interatomic entanglement of the spins in the chain, demonstrating the prerequisites to build and probe spatially extended strongly correlated nanostructures., D.J.C. and J.A.J.B. acknowledge postdoctoral fellowship from the Alexander von Humboldt foundation. M.T. acknowledges support from the DFG-SFB 767. J.A.J.B. acknowledges support from the Natural Sciences and Engineering Research Council of Canada. N.L. and R.R. acknowledge support form Spanish MINECO (grant no. MAT2012-38318-C03-02 with joint financing by FEDER Funds from the European Union). ICN2 acknowledges support from the Severo Ochoa Program (MINECO, grant SEV-2013-0295).

Scattering of electrons by localized spins is the ultimate process enabling detection and control of the magnetic state of a spin-doped material. At the molecular scale, scattering is mediated by the orbitals hosting the spin. Here we report the selective excitation of a molecular spin by tunneling through different molecular orbitals. Spatially resolved tunneling spectra on iron-porphyrins reveal that the inelastic spin excitation extends beyond the iron site, changing shape and symmetry along the molecule. Combining density functional theory simulations with a phenomenological scattering model, we show that the extension and lineshape of the inelastic signal are due to excitation pathways assisted by different frontier orbitals. By selecting the intramolecular site for electron injection, the relative weight of iron and pyrrole orbitals in the tunneling process is modified. Thus, the excitation mechanism, reflected by its spectral lineshape, depends on the degree of localization and energy alignment of the chosen molecular orbital., This work has been funded by the COST 15128 Molecular Spintronics project, by Marie Curie IF ARTE, by the Spanish Ministerio de Economía y Competitividad (MINECO) through the cooperative grant No. MAT2016-78293 and grant No. FIS2016-75862-P, and by the Basque Government (Dep. Industry, Grant PI-2015-1-42, Dep. Education, Grant PI-2016-1-27 and Grant IT-756-13), the EU project PAMS (610446), and the European Regional Development Fund (ERDF).

A low-temperature scanning tunneling microscope was employed to study the differential conductance in an atomic junction formed by an adsorbed Co atom on a Cu(100) surface and a copper-covered tip. A zero-bias anomaly (ZBA) reveals spin scattering off the Co atom, which is assigned to a Kondo effect. The ZBA exhibits a characteristic asymmetric lineshape when electrons tunnel between tip and sample, while upon the tip-Co contact it symmetrizes and broadens. Through density functional theory calculations and the non-equilibrium non-crossing approximation, we show that the lineshape broadening is mainly a consequence of the additional coupling to the tip, while non-equilibrium effects only modify the large-bias tails of the ZBA., D.J.C. acknowledges the European Union for support under H2020-MSCA-IF-2014 Marie-Curie Individual Fellowship programme Proposal No. 654469. P.A. acknowledges the CCT-Rosario Computational Center. Financial support from CONICET, the Agence Nationale de la Recherche (Grant Nos. ANR-13-BS10-0016, ANR-11-LABX-0058 NIE, and ANR-10-LABX-0026 CSC), and MINECO (Grant No. MAT2015-66888-C3-2-R) is gratefully acknowledged.

The Kondo effect of a Co atom on Cu(100) was investigated with a low-temperature scanning tunneling microscope using a monoatomically sharp nickel tip. Upon a tip-Co contact, the differential conductance spectra exhibit a spin-split asymmetric Kondo resonance. The computed ab initio value of the exchange coupling is too small to suppress the Kondo effect, but sufficiently large to produce the splitting observed. A quantitative analysis of the line shape using the numerical renormalization group technique indicates that the junction spin polarization is weak., 5 pages, 4 figures

Heterogeneous atomic magnetic chains are built by atom manipulation on a ${\mathrm{Cu}}_{2}\mathrm{N}/\mathrm{Cu}$ (100) substrate. Their magnetic properties are studied and rationalized by a combined scanning tunneling microscopy (STM) and density functional theory (DFT) work completed by model Hamiltonian studies. The chains are built using Fe and Mn atoms ontop of the Cu atoms along the N rows of the ${\mathrm{Cu}}_{2}\mathrm{N}$ surface. Here, we present results for ${\mathrm{FeMn}}_{x}$ chains $(x=1--6)$ emphasizing the evolution of the geometrical, electronic, and magnetic properties with chain size. By fitting our results to a Heisenberg Hamiltonian we have studied the exchange-coupling matrix elements $J$ for different chains. For the shorter chains, $x\ensuremath{\le}2$, we have included spin-orbit effects in the DFT calculations, extracting the magnetic anisotropy energy. Our results are also fitted to a simple anisotropic spin Hamiltonian and we have extracted values for the longitudinal-anisotropy $D$ and transversal-anisotropy $E$ constants. These parameters together with the values for $J$ allow us to compute the magnetic excitation energies of the system and to compare them with the experimental data.

Scanning tunnelling microscopy and density functional theory studies of manganese chains adsorbed on CuN/Cu (100) reveal an unsuspected electronic edge state at ∼ 1 eV above the Fermi energy. This Tamm-like state is strongly localised to the terminal Mn atoms of the chain and fully spin polarised. However, no equivalence is found for occupied states, and the electronic structure at ∼ -1 eV is mainly spin unpolarised due to the extended p-states of the N atoms that mediate the coupling between the Mn atoms in the chain. The spin polarisation of the edge state is affected by the antiferromagnetic ordering of the chains leading to non-trivial consequences., We acknowledge the European Union for support under the Marie-Skłodowska Curie Program through IF (DJC) and CIG (JIP) grants. We also acknowledge support from MINECO via grants MAT2015-66888-C3-2-R (NL), MAT2013-46593-C6-01 (JIP) and Severo Ochoa Program grant SEV-2013-0295 (ICN2).

Spin polarized tunneling through a hybrid tunnel barrier of a Spin filter (SF) based on a EuO ferro-magnetic semiconductor and an organic semiconductor (OSC) (rubrene in this case) was investigated. For quasi-magnetic tunnel junction (MTJ) structures, such as Co/rubrene/EuO/Al, we observed a strong spin filtering effect of the EuO layer exhibiting I-V curves with high spin polarization (P) of up to 99% measured at 4 K. However, a magnetoresistance (MR) value of 9% was obtained at 4.2 K. The low MR compared to the high P could be attributed to spin scattering caused by structural defects at the interface between the EuO and rubrene, due to nonstoichiometry in the EuO.

Weexploitseveralscanningtunnelingmicroscopy(STM)techniques, such as atom manipulated scans and constant-height scans, to atomically resolve the adsorption geometry of isolated cobalt-phthalocyanine (CoPc) molecules on a copper (111) surface and to obtain proper low-temperature maps of the molecular conductance. By comparing these crucial findings to density functional calcula- tions, we then provide fresh insight into the CoPc-metal interface. This innovative STM study should be applicable to a wide variety of molecules relevant for mole- cular electronics. SECTION Surfaces, Interfaces, Catalysis

Recently a memristor ( Chua, L. O. IEEE Trans. Circuit Theory 1971 , 18 , 507 ), the fourth fundamental passive circuit element, has been demonstrated as thin film device operations ( Strukov, D. B.; Snider, G. S.; Stewart, D. R.; Williams, R. S. Nature (London) 2008 , 453 , 80 ; Yang, J. J.; Pickett. M. D.; Li, X.; Ohlberg, D. A. A.; Stewart, D. R.; Williams, R. S. Nat. Nanotechnol. 2008 , 3 , 429 ). A new addition to the memristor family can be nanoparticle assemblies consisting of an infinite number of monodispersed, crystalline magnetite (Fe(3)O(4)) particles. Assembly of nanoparticles that have sizes below 10 nm, exhibits at room temperature a voltage-current hysteresis with an abrupt and large bipolar resistance switching (R(OFF)/R(ON) approximately 20). Interestingly, observed behavior could be interpreted by adopting an extended memristor model that combines both a time-dependent resistance and a time-dependent capacitance. We also observed that such behavior is not restricted to magnetites; it is a general property of nanoparticle assemblies as it was consistently observed in different types of spinel structured nanoparticles with different sizes and compositions. Further investigation into this new nanoassembly system will be of importance to the realization of the next generation nanodevices with potential advantages of simpler and inexpensive device fabrications.

Magnetite() is currently one of key materials for applications in magnetic storage and many bioinspired applications because bulk has a high Curie temperature($Tc

Magnetic anisotropy plays a key role in the magnetic stability and spin-related quantum phenomena of surface adatoms. It manifests as angular variations of the atom's magnetic properties. We measure the spin excitations of individual Fe atoms on a copper nitride surface with inelastic electron tunneling spectroscopy. Using a three-axis vector magnet we rotate the magnetic field and map out the resulting variations of the spin excitations. We quantitatively determine the three-dimensional distribution of the magnetic anisotropy of single Fe atoms by fitting the spin excitation spectra with a spin Hamiltonian. This experiment demonstrates the feasibility of fully mapping the vector magnetic properties of individual spins and characterizing complex three-dimensional magnetic systems.

A low-temperature scanning tunneling microscope is employed to build a junction comprising a Co atom bridging a copper-coated tip and a Cu(100) surface. An Abrikosov-Suhl-Kondo resonance is evidenced in the differential conductance and its width is shown to vary exponentially with the ballistic conductance for all tips employed. Using a theoretical description based on the Anderson model, we show that the Kondo effect and the total conductance are related through the atomic relaxations affecting the environment of the Co atom. Erratum in : Phys Rev Lett. 2012 Oct 12;109(15):159901.

Low-temperature scanning tunneling microscopy and spectroscopy are employed to investigate electron tunneling from a C60-terminated tip into a Cu(111) surface. Tunneling between a C60 orbital and the Shockley surface states of copper is shown to produce negative differential conductance (NDC) contrary to conventional expectations. NDC can be tuned through barrier thickness or C60 orientation up to complete extinction. The orientation dependence of NDC is a result of a symmetry matching between the molecular tip and the surface states., 5 pages, 4 figures, 1 table

Turning graphene magnetic is a promising challenge to make it an active material for spintronics. Predictions state that graphene structures with specific shapes can spontaneously develop magnetism driven by Coulomb repulsion of π-electrons, but its experimental verification is demanding. Here, we report on the observation and manipulation of individual magnetic moments in graphene open-shell nanostructures on a gold surface. Using scanning tunneling spectroscopy, we detect the presence of single electron spins localized around certain zigzag sites of the carbon backbone via the Kondo effect. We find near-by spins coupled into a singlet ground state and quantify their exchange interaction via singlet-triplet inelastic electron excitations. Theoretical simulations picture how electron correlations result in spin-polarized radical states with the experimentally observed spatial distributions. Extra hydrogen atoms bound to radical sites quench their magnetic moment and switch the spin of the nanostructure in half-integer amounts. Our work demonstrates the intrinsic π-paramagnetism of graphene nanostructures.

Turning graphene magnetic is a promising challenge to make it an active material for spintronics. Predictions state that graphene structures with specific shapes can spontaneously develop magnetism driven by Coulomb repulsion of π-electrons, but its experimental verification is demanding. Here, we report on the observation and manipulation of individual magnetic moments in graphene open-shell nanostructures on a gold surface. Using scanning tunneling spectroscopy, we detect the presence of single electron spins localized around certain zigzag sites of the carbon backbone via the Kondo effect. We find near-by spins coupled into a singlet ground state and quantify their exchange interaction via singlet-triplet inelastic electron excitations. Theoretical simulations picture how electron correlations result in spin-polarized radical states with the experimentally observed spatial distributions. Extra hydrogen atoms bound to radical sites quench their magnetic moment and switch the spin of the nanostructure in half-integer amounts. Our work demonstrates the intrinsic π-paramagnetism of graphene nanostructures.