Advanced capabilities for materials modelling with Quantum ESPRESSO.

Quantum EXPRESSO is an integrated suite of open-source computer codes for quantum simulations of materials using state-of-the-art electronic-structure techniques, based on density-functional theory, density-functional perturbation theory, and many-body perturbation theory, within the plane-wave pseudopotential and projector-augmented-wave approaches. Quantum EXPRESSO owes its popularity to the wide variety of properties and processes it allows to simulate, to its performance on an increasingly broad array of hardware architectures, and to a community of researchers that rely on its capabilities as a core open-source development platform to implement their ideas. In this paper we describe recent extensions and improvements, covering new methodologies and property calculators, improved parallelization, code modularization, and extended interoperability both within the distribution and with external software.

Tuning the Magnetic Anisotropy at a Molecule-Metal Interface.

We demonstrate that a C(60) overlayer enhances the perpendicular magnetic anisotropy of a Co thin film, inducing an inverse spin reorientation transition from in plane to out of plane. The driving force is the (60)/Co interfacial magnetic anisotropy that we have measured quantitatively in situ as a function of the (60) coverage. Comparison with state-of-the-art ab initio calculations show that this interfacial anisotropy mainly arises from the local hybridization between (60) p(z) and Co d(z(2)) orbitals. By generalizing these arguments, we also demonstrate that the hybridization of (60) with a Fe(110) surface decreases the perpendicular magnetic anisotropy. These results open the way to tailor the interfacial magnetic anisotropy in organic-material-ferromagnet systems.

Electronic and magnetic structure of the Cr(001) surface.

Density functional theory (DFT) calculations are carried out to study the electronic and magnetic structure of the (001) surface of chromium. Our aim is to identify and characterize the most prominent electronic surface states and make the connection with the main experimental results. We show that a low dispersive minority spin surface state at the center of the surface Brillouin zone plays a crucial role. This surface state of Δ1 symmetry at 0.58 eV above the Fermi level exhibits a predominantly dz(2) as well as pz orbital character. Local density of states (LDOS) analysis in the vacuum above the surface shows that the sharp feature originating from this surface state persists far away above the surface because of the slow decay rate of the pz wavefunction. Finally, by artificially lowering the surface magnetic moment [Formula: see text] on the outermost surface layer we find excellent agreement with experiments for [Formula: see text]. In addition, we propose that some extra spin polarized scanning tunneling spectroscopy (SP-STS) experiments should be made at smaller tip-surface distances to reveal additional features originating from the majority spin dz(2) surface state.

Kondo effect of magnetic impurities in nanotubes.

Transition metal impurities will yield zero-bias anomalies in the conductance of well contacted metallic carbon nanotubes, but Kondo temperatures and geometry dependences have not been anticipated so far. Applying the density functional plus numerical renormalization group approach of Lucignano et al. to Co and Fe impurities in (4,4) and (8,8) nanotubes, we discover a huge difference of behavior between outside versus inside adsorption of the impurity. The predicted Kondo temperatures and zero-bias anomalies, tiny outside the nanotube, turn large and strongly radius dependent inside, owing to a change of symmetry of the magnetic orbital. Observation of this Kondo effect should open the way to a host of future experiments.

Large magnetoresistance through a single molecule due to a spin-split hybridized orbital.

Using organic materials in spintronic devices raises a lot of expectation for future applications due to their flexibility, low cost, long spin lifetime, and easy functionalization. However, the interfacial hybridization and spin polarization between the organic layer and the ferromagnetic electrodes still has to be understood at the molecular scale. Coupling state-of-the-art spin-polarized scanning tunneling spectroscopy and spin-resolved ab initio calculations, we give the first experimental evidence of the spin splitting of a molecular orbital on a single non magnetic C(60) molecule in contact with a magnetic material, namely, the Cr(001) surface. This hybridized molecular state is responsible for an inversion of sign of the tunneling magnetoresistance depending on energy. This result opens the way to spin filtering through molecular orbitals.

Colossal magnetic anisotropy of monatomic free and deposited platinum nanowires.

Whenever a nanosystem such as an adatom, a cluster or a nanowire spontaneously magnetizes, a crucial parameter is its magnetic anisotropy, the intrinsic preference of magnetization to lie along an easy axis. Anisotropy is important in nanosystems because it helps reduce the magnitude of thermal (superparamagnetic) fluctuations, it can modify the flow of current, and it can induce new phenomena, such as the quantum tunnelling of magnetization. We discuss here, on the basis of density functional calculations, the novel and unconventional feature of colossal magnetic anisotropy--the strict impossibility of magnetization to rotate from the parallel to the orthogonal direction--which, owing to a quantum mechanical selection rule, the recently predicted Pt nanowire magnetism should exhibit. Model calculations suggest that the colossal magnetic anisotropy of a Pt chain should persist after weak adsorption on an inert substrate or surface step.