Dimensionality driven charge density wave instability in TiS$_2$

Density functional theory and density functional perturbation theory are used to investigate the electronic and vibrational properties of TiS$_2$. Within the local density approximation the material is a semi-metal both in the bulk and in the monolayer form. Most interestingly we observe a Kohn anomaly in the bulk phonon dispersion, which turns into a charge density wave instability when TiS$_2$ is thinned to less than four monolayers. Such charge density wave phase can be tuned by compressive strain, which appears to be the control parameter of the instability.

Detection of the electrostatic spin crossover effect in magnetic molecules

Scanning tunneling microscopy (STM) can be used to detect inelastic spin transitions in magnetic nano-structures comprising only a handful of atoms. Here we demonstrate that STM can uniquely identify the electrostatic spin crossover effect, whereby the exchange interaction between two magnetic centers in a magnetic molecule changes sign as a function of an external electric field. The fingerprint of such effect is a large drop in the differential conductance as the bias increases. Crucially in the case of a magnetic dimer the spin crossover transition inverts the order between the ground state and the first excited state, but does not change their symmetry. This means that at both sides of the conductance drop associated to the spin crossover transition there are two inelastic transition between the same states. The corresponding conductance steps split identically in a magnetic field and provide a unique way to identify the electrostatic spin crossover.

Persistent current and Drude weight for the one-dimensional Hubbard model from current lattice density functional theory

The Bethe-Ansatz local density approximation (LDA) to lattice density functional theory (LDFT) for the one-dimensional repulsive Hubbard model is extended to current-LDFT (CLDFT). The transport properties of mesoscopic Hubbard rings threaded by a magnetic flux are then systematically investigated by this scheme. In particular we present calculations of ground state energies, persistent currents and Drude weights for both a repulsive homogeneous and a single impurity Hubbard model. Our results for the ground state energies in the metallic phase compares favorably well with those obtained with numerically accurate many-body techniques. Also the dependence of the persistent currents on the Coulomb and the impurity interaction strength, and on the ring size are all well captured by LDA-CLDFT. Our study demonstrates that CLDFT is a powerful tool for studying one-dimensional correlated electron systems with high accuracy and low computational costs.

Monte-Carlo phase diagram of a Hubbard-Peierls model in the search for spin crossover transition in $pi$-conjugated polymers

We present a Monte Carlo study of the finite temperature properties of an extended Hubbard-Peierls model describing one dimensional $pi$-conjugated polymers. The model incorporates electron-phonon and hyperfine interaction and it is solved at the mean field level for half filling. In particular we explore the model as a function of the strength of electron-electron and electron-phonon interactions. At low temperature the system presents a diamagnetic to antiferromagnetic transition as the electron-electron interaction strength increases. At the same time by increasing the electron-phonon coupling there is a transition from a homogeneous to a Peierls dimerized geometry. As expected such a Peierls dimerized phase disappears at finite temperature as a result of thermal vibrations. More intriguing is the interplay between the electron-phonon and the electron-electron interactions at finite temperature. In particular we demonstrate that for a certain region of the parameter space there is a spin-crossover, where the system transits from a low-spin to a high-spin state as the temperature increases. In close analogy to standard spin-crossover in divalent magnetic molecules such a transition is entropy driven. Finally we discuss the role played by the hyperfine interaction over the phase diagram.

The magnetism of wurtzite CoO nanoclusters

The possibility that the apparent room temperature ferromagnetism, often measured in Co-doped ZnO, is due to uncompensated spins at the surface of wurtzite CoO nanoclusters is investigated by means of a combination of density functional theory and Monte Carlo simulations. We find that the critical temperature extracted from the specific heat systematically drops as the cluster size is reduced, regardless of the particular cluster shape. Furthermore the presence of defects, in the form of missing magnetic sites, further reduces $T_mathrm{C}$. This suggests that even a spinodal decomposed phase is unlikely to sustain room temperature ferromagnetism in ZnO:Co.

Electron transport across electrically switchable magnetic molecules

We investigate the electron transport properties of a model magnetic molecule formed by two magnetic centers whose exchange coupling can be altered with a longitudinal electric field. In general we find a negative differential conductance at low temperatures originating from the different scattering amplitudes of the singlet and triplet states. More interestingly, when the molecule is strongly coupled to the leads and the potential drop at the magnetic centers is only weakly dependent on the magnetic configuration, we find that there is a critical voltage V_C at which the current becomes independent of the temperature. This corresponds to a peak in the low temperature current noise. In such limit we demonstrate that the quadratic current fluctuations are proportional to the product between the conductance fluctuations and the temperature.

Impurity-Ion pair induced high-temperature ferromagnetism in Co-doped ZnO

Magnetic 3d-ions doped into wide-gap oxides show signatures of room temperature ferromagnetism, although their concentration is two orders of magnitude smaller than that in conventional magnets. The prototype of these exceptional materials is Co-doped ZnO, for which an explanation of the room temperature ferromagnetism is still elusive. Here we demonstrate that magnetism originates from Co2+ oxygen-vacancy pairs with a partially filled level close to the ZnO conduction band minimum. The magnetic interaction between these pairs is sufficiently long-ranged to cause percolation at moderate concentrations. However, magnetically correlated clusters large enough to show hysteresis at room temperature already form below the percolation threshold and explain the current experimental findings. Our work demonstrates that the magnetism in ZnO:Co is entirely governed by intrinsic defects and a phase diagram is presented. This suggests a recipe for tailoring the magnetic properties of spintronics materials by controlling their intrinsic defects.