Spin alignment of extra electrons in K-phenanthrene clusters taken from the crystalline tripotassium-intercalated phenanthrene structure

The appearance of ferromagnetic correlations among π electrons of phenanthrene (C14H10) molecules in the herringbone structure is proven for K doped clusters both by ab initio quantum-chemistry calculations and by the direct solution of the many-body Pariser-Parr-Pople Hamiltonian. Magnetic ground states are predicted for one or three additional electrons per phenanthrene molecule. These results are a consequence of the small overlap between the lowest unoccupied molecular orbitals (and lowest unoccupied molecular orbitals + 1) of neutral neighboring phenanthrene molecules, which makes the gain in energy by delocalization similar to the corresponding increase due to the Coulomb interaction.

Graphene single-electron transistor as a spin sensor for magnetic adsorbates

We study single-electron transport through a graphene quantum dot with magnetic adsorbates. We focus on the relation between the spin order of the adsorbates and the linear conductance of the device. The electronic structure of the graphene dot with magnetic adsorbates is modeled through numerical diagonalization of a tight-binding model with an exchange potential. We consider several mechanisms by which the adsorbate magnetic state can influence transport in a single-electron transistor: tuning the addition energy, changing the tunneling rate, and in the case of spin-polarized electrodes, through magnetoresistive effects. Whereas the first mechanism is always present, the others require that the electrode has to have either an energy- or spin-dependent density of states. We find that graphene dots are optimal systems to detect the spin state of a few magnetic centers.

Exponential decay of spin-spin correlation between distant defect states produced by contour hydrogenation of polycyclic aromatic hydrocarbon molecules

The first few low-lying spin states of alternant polycyclic aromatic hydrocarbon (PAH) molecules of several shapes showing defect states induced by contour hydrogenation have been studied both by ab initio methods and by a precise numerical solution of Pariser-Parr-Pople (PPP) interacting model. In accordance with Lieb's theorem, the ground state shows a spin multiplicity equal to one for balanced molecules, and it gets larger values for imbalanced molecules (that is, when the number of π electrons on both subsets is not equal). Furthermore, we find a systematic decrease of the singlet-triplet splitting as a function of the distance between defects, regardless of whether the ground state is singlet or triplet. For example, a splitting smaller than 0.001 eV is obtained for a medium size C46H28 PAH molecule (di-hydrogenated [11]phenacene) showing a singlet ground state. We conclude that π electrons unbound by lattice defects tend to remain localized and unpaired even when long-range Coulomb interaction is taken into account. Therefore they show a biradical character (polyradical character for more than two defects) and should be studied as two or more local doublets. The implications for electron transport are potentially important since these unpaired electrons can trap traveling electrons or simply flip their spin at a very small energy cost.

Intrinsic spin noise in MgO magnetic tunnel junctions

We consider two intrinsic sources of noise in ultra-sensitive magnetic field sensors based on MgO magnetic tunnel junctions, coming both from 25 Mg nuclear spins (I = 5/2, 10% natural abundance) and S = 1 Mg-vacancies. While nuclear spins induce noise peaked in the MHz frequency range, the vacancies noise peaks in the GHz range. We find that the nuclear noise in submicron devices has a similar magnitude than the 1/f noise, while the vacancy-induced noise dominates in the GHz range. Interestingly, the noise spectrum under a finite magnetic field gradient may provide spatial information about the spins in the MgO layer.

A highly resistive layer within the crust of X-ray pulsars limits their spin periods

The lack of isolated X-ray pulsars with spin periods longer than 12 s raises the question of where the population of evolved high-magnetic-field neutron stars has gone. Unlike canonical radiopulsars, X-ray pulsars are not subject to physical limits to the emission mechanism nor observational biases against the detection of sources with longer periods. Here we show that a highly resistive layer in the innermost part of the crust of neutron stars naturally limits the spin period to a maximum value of about 10–20 s. This highly resistive layer is expected if the inner crust is amorphous and heterogeneous in nuclear charge, possibly owing to the existence of a nuclear ‘pasta’ phase. Our findings suggest that the maximum period of isolated X-ray pulsars may be the first observational evidence for an amorphous inner crust, whose properties can be further constrained by future X-ray timing missions combined with more detailed models.

Local probe of fractional edge states of S=1 Heisenberg spin chains

Spin chains are among the simplest physical systems in which electron-electron interactions induce novel states of matter. Here we propose to combine atomic scale engineering and spectroscopic capabilities of state of the art scanning tunnel microscopy to probe the fractionalized edge states of individual atomic scale S=1 spin chains. These edge states arise from the topological order of the ground state in the Haldane phase. We also show that the Haldane gap and the spin-spin correlation length can be measured with the same technique.

Cyclobutadiene automerization and rotation of ethylene: Energetics of the barriers by using Spin-polarized wave functions

Spin-projected spin polarized Møller–Plesset and spin polarized coupled clusters calculations have been made to estimate the cyclobutadiene automerization, the ethylene torsion barriers in their ground state, and the gap between the singlet and triplet states of ethylene. The results have been obtained optimizing the geometries at MP4 and/or CCSD levels, by an extensive Gaussian basis set. A comparative analysis with more complex calculations, up to MP5 and CCSDTQP, together with others from the literature, have also been made, showing the efficacy of using spin-polarized wave functions as a reference wave function for Møller–Plesset and coupled clusters calculations, in such problems.

Orbital Magnetization of Quantum Spin Hall Insulator Nanoparticles

Both spin and orbital degrees of freedom contribute to the magnetic moment of isolated atoms. However, when inserted in crystals, atomic orbital moments are quenched because of the lack of rotational symmetry that protects them when isolated. Thus, the dominant contribution to the magnetization of magnetic materials comes from electronic spin. Here we show that nanoislands of quantum spin Hall insulators can host robust orbital edge magnetism whenever their highest occupied Kramers doublet is singly occupied, upgrading the spin edge current into a charge current. The resulting orbital magnetization scales linearly with size, outweighing the spin contribution for islands of a few nm in size. This linear scaling is specific of the Dirac edge states and very different from Schrodinger electrons in quantum rings. By modeling Bi(111) flakes, whose edge states have been recently observed, we show that orbital magnetization is robust with respect to disorder, thermal agitation, shape of the island, and crystallographic direction of the edges, reflecting its topological protection.

Imaging of spin waves in atomically designed nanomagnets

The spin dynamics of all ferromagnetic materials are governed by two types of collective phenomenon: spin waves and domain walls. The fundamental processes underlying these collective modes, such as exchange interactions and magnetic anisotropy, all originate at the atomic scale. However, conventional probing techniques based on neutron1 and photon scattering2 provide high resolution in reciprocal space, and thereby poor spatial resolution. Here we present direct imaging of standing spin waves in individual chains of ferromagnetically coupled S = 2 Fe atoms, assembled one by one on a Cu2N surface using a scanning tunnelling microscope. We are able to map the spin dynamics of these designer nanomagnets with atomic resolution in two complementary ways. First, atom-to-atom variations of the amplitude of the quantized spin-wave excitations are probed using inelastic electron tunnelling spectroscopy. Second, we observe slow stochastic switching between two opposite magnetization states3, 4, whose rate varies strongly depending on the location of the tip along the chain. Our observations, combined with model calculations, reveal that switches of the chain are initiated by a spin-wave excited state that has its antinodes at the edges of the chain, followed by a domain wall shifting through the chain from one end to the other. This approach opens the way towards atomic-scale imaging of other types of spin excitation, such as spinon pairs and fractional end-states5, 6, in engineered spin chains.

Derivation of the spin Hamiltonians for Fe in MgO

A method to calculate the effective spin Hamiltonian for a transition metal impurity in a non-magnetic insulating host is presented and applied to the paradigmatic case of Fe in MgO. In the first step we calculate the electronic structure employing standard density functional theory (DFT), based on generalized gradient approximation (GGA), using plane waves as a basis set. The corresponding basis of atomic-like maximally localized Wannier functions is derived and used to represent the DFT Hamiltonian, resulting in a tight-binding model for the atomic orbitals of the magnetic impurity. The third step is to solve, by exact numerical diagonalization, the N electron problem in the open shell of the magnetic atom, including both effects of spin–orbit and Coulomb repulsion. Finally, the low energy sector of this multi-electron Hamiltonian is mapped into effective spin models that, in addition to the spin matrices S, can also include the orbital angular momentum L when appropriate. We successfully apply the method to Fe in MgO, considering both the undistorted and Jahn–Teller (JT) distorted cases. Implications for the influence of Fe impurities on the performance of magnetic tunnel junctions based on MgO are discussed.

Controlled Complete Suppression of Single-Atom Inelastic Spin and Orbital Cotunneling

The inelastic portion of the tunnel current through an individual magnetic atom grants unique access to read out and change the atom’s spin state, but it also provides a path for spontaneous relaxation and decoherence. Controlled closure of the inelastic channel would allow for the latter to be switched off at will, paving the way to coherent spin manipulation in single atoms. Here, we demonstrate complete closure of the inelastic channels for both spin and orbital transitions due to a controlled geometric modification of the atom’s environment, using scanning tunneling microscopy (STM). The observed suppression of the excitation signal, which occurs for Co atoms assembled into chains on a Cu2N substrate, indicates a structural transition affecting the dz2 orbital, effectively cutting off the STM tip from the spin-flip cotunneling path.