Designing a molecular magnetic button based on 4d and 5d transition-metal phthalocyanines.

The field of molecular spintronics exploits the properties of organic molecules possessing a magnetic moment, either native in the form of radicals or induced by the insertion of transition metal magnetic ions. To realize logic or storage molecular spin-tronics devices, molecules with stable different magnetic states should be deposited on a substrate, and switching between the states controllably achieved. By means of a first-principles calculations, we have devised a functional molecule exhibiting different magnetic states upon structural changes induced by current injection. We investigate the prototypical case of non-planar M-Phthalocyanine (MPc), where M is a transition-metal ion belonging to the 4d and 5d series. We find that for ZrPc and HfPc deposited on a graphene decorated Ni(111) substrate, two different structural conformations could be stabilized, for which the molecules attain different magnetic states depending on the position of the M ion - whether above the Pc or between the Pc and the substrate -, acting therefore as molecular magnetic button. Our work indicates an intuitive way to engineer a magnetic molecular switch with tailored properties, starting from the knowledge of the basic atomic properties of elements and surfaces.

Tunneling anisotropic magnetoresistance at the single-atom limit.

The tunneling anisotropic magnetoresistance (TAMR) of single Co atoms adsorbed on a double-layer Fe film on W(110) is observed by scanning tunneling spectroscopy. Without applying an external magnetic field the TAMR is found by comparing spectra of atoms that are adsorbed on the domains and domain walls of the Fe film. The TAMR can be as large as 12% and repeatedly changes sign as a function of bias voltage. First-principles calculations show that the hybridization between Co d states of different orbital symmetries depends on the magnetization direction via spin-orbit coupling. This leads to an anisotropy of the density of states and thus induces a TAMR.

Conical spin-spiral state in an ultrathin film driven by higher-order spin interactions.

We report a transverse conical spin spiral as the magnetic ground state of a double-layer Mn on a W(110) surface. Using spin-polarized scanning tunneling microscopy, we find a long-range modulation along the [001] direction with a periodicity of 2.4 nm coexisting with a local row-wise antiferromagnetic contrast. First-principles calculations reveal a transverse conical spin-spiral ground state of this system which explains the observed magnetic contrast. The canting of the spins is induced by higher-order exchange interactions, while the spiraling along the [001] direction is due to frustrated Heisenberg exchange and Dzyaloshinskii-Moriya interaction.

Atomic-scale spin spiral with a unique rotational sense: Mn monolayer on W(001).

Using spin-polarized scanning tunneling microscopy we show that the magnetic order of 1 monolayer Mn on W(001) is a spin spiral propagating along 110 crystallographic directions. The spiral arises on the atomic scale with a period of about 2.2 nm, equivalent to only 10 atomic rows. Ab initio calculations identify the spin spiral as a left-handed cycloid stabilized by the Dzyaloshinskii-Moriya interaction, imposed by spin-orbit coupling, in the presence of softened ferromagnetic exchange coupling. Monte Carlo simulations explain the formation of a nanoscale labyrinth pattern, originating from the coexistence of the two possible rotational domains, that is intrinsic to the system.

Magnetic phase control in monolayer films by substrate tuning.

We propose tailoring exchange interactions in magnetic monolayer films by tuning the adjacent nonmagnetic substrate. As an example, we demonstrate a ferromagnetic-antiferromagnetic phase transition for one monolayer Fe on a Ta(x)W(1-x)(001) surface as a function of the Ta concentration. At the critical Ta concentration, the nearest-neighbor exchange interaction is small and the magnetic phase space is dramatically broadened. Complex magnetic order such as spin spirals, multiple-Q, or even disordered local moment states can occur, offering the possibility of storing information in terms of ferromagnetic dots in an otherwise zero-magnetization state matrix.

Chiral magnetic order at surfaces driven by inversion asymmetry.

Chirality is a fascinating phenomenon that can manifest itself in subtle ways, for example in biochemistry (in the observed single-handedness of biomolecules) and in particle physics (in the charge-parity violation of electroweak interactions). In condensed matter, magnetic materials can also display single-handed, or homochiral, spin structures. This may be caused by the Dzyaloshinskii-Moriya interaction, which arises from spin-orbit scattering of electrons in an inversion-asymmetric crystal field. This effect is typically irrelevant in bulk metals as their crystals are inversion symmetric. However, low-dimensional systems lack structural inversion symmetry, so that homochiral spin structures may occur. Here we report the observation of magnetic order of a specific chirality in a single atomic layer of manganese on a tungsten (110) substrate. Spin-polarized scanning tunnelling microscopy reveals that adjacent spins are not perfectly antiferromagnetic but slightly canted, resulting in a spin spiral structure with a period of about 12 nm. We show by quantitative theory that this chiral order is caused by the Dzyaloshinskii-Moriya interaction and leads to a left-rotating spin cycloid. Our findings confirm the significance of this interaction for magnets in reduced dimensions. Chirality in nanoscale magnets may play a crucial role in spintronic devices, where the spin rather than the charge of an electron is used for data transmission and manipulation. For instance, a spin-polarized current flowing through chiral magnetic structures will exert a spin-torque on the magnetic structure, causing a variety of excitations or manipulations of the magnetization and giving rise to microwave emission, magnetization switching, or magnetic motors.

Atomic spin structure of antiferromagnetic domain walls.

The search for uncompensated magnetic moments on antiferromagnetic surfaces is of great technological importance as they are responsible for the exchange-bias effect that is widely used in state-of-the-art magnetic storage devices. We have studied the atomic spin structure of phase domain walls in the antiferromagnetic Fe monolayer on W(001) by means of spin-polarized scanning tunnelling microscopy and Monte Carlo simulations. The domain wall width only amounts to 6-8 atomic rows. Although walls oriented along <100> directions are found to be fully compensated, detailed analysis of <110>-oriented walls reveals an uncompensated perpendicular magnetic moment. Our result represents a major advance in the field of antiferromagnetism, and may lead to a better understanding of the magnetic interaction between ferromagnetic and antiferromagnetic materials.

Revealing antiferromagnetic order of the Fe monolayer on W(001): spin-polarized scanning tunneling microscopy and first-principles calculations.

We prove that the magnetic ground state of a single monolayer Fe on W(001) is c(2x2) antiferromagnetic, i.e., a checkerboard arrangement of antiparallel magnetic moments. Real space images of this magnetic structure have been obtained with spin-polarized scanning tunneling microscopy. An out-of-plane easy magnetization axis is concluded from measurements in an external magnetic field. The magnetic ground state and anisotropy axis are explained based on first-principles calculations.