Ab initiodescription of disorder effects in layered cathode active materials by the coherent potential approximation.

Disorder effects in alloys are usually modeled by averaging various supercell calculations considering different positions of the alloy atoms. This approach, however, is only possible as long as the portion of the individual components of the alloy is sufficiently large. Herein, we present anab initiostudy considering the lithium insertion material Li1-x[Ni0.33Co0.33Mn0.33]O2as model system to demonstrate the power of the coherent potential approximation within the Korringa-Kohn-Rostoker Green's function method. This approach enables the description of disorder effects within alloy systems of any composition. It is applied in this study to describe the (de-)intercalation of arbitrary amounts of lithium from the cathode active material. Moreover, we highlight that using either fully optimized structures or experimental lattice parameters and atomic positions both lead to comparable results. Our findings suggest that this approach is also suitable for modeling the electronic structure of state-of-the-art materials such as high-nickel alloys.

Ab initio calculations of conduction band effective mass parameters of thermoelectric [Formula: see text] (X, Y = Si, Ge, Sn) alloys.

Since there are still research interests in the physical properties of quasi-binary thermoelectric [Formula: see text] alloys, with X, Y = Si, Ge, Sn, we present an ab initio analysis that yields the relative formation energy and effective masses of the conduction bands, in the whole compositional range x. We base our calculations on the full-relativistic Korringa, Kohn and Rostocker (KKR) Green's functions formalism within the coherent potential approximation (CPA). Formation energies, measured relative to the end [Formula: see text] compounds, show no excess energy for the [Formula: see text] substitution thus indicating a complete solubility. In contrast, concave and asymmetric formation energies for intermediate compositions in the [Formula: see text] alloys manifest a miscibility gap. With this basis, we compute and discuss the crossing of the conduction bands observed in n-type [Formula: see text] materials. We present direction- and band-dependent effective masses using a generalized single parabolic band effective mass approximation to discuss anisotropic effects, to interpret available experimental and theoretical data, and to predict intermediate and not yet published transport parameters on these alloys.

Thermal Transport and Nonequilibrium Temperature Drop Across a Magnetic Tunnel Junction.

In the field of spin caloritronics, spin-dependent transport phenomena are observed in a number of current experiments where a temperature gradient across a nanostructured interface is applied. The interpretation of these experiments is not clear as both phonons and electrons may contribute to thermal transport. Therefore, it still remains an open question how the temperature drop across a magnetic nanostructured interface arises microscopically. We answer this question for the case of a magnetic tunnel junction (MTJ) where the tunneling magneto-Seebeck effect occurs. Our explanation may be extended to other types of nanostructured interfaces. We explicitly calculate phonon and electron thermal conductance across Fe/MgO/Fe MTJs in an ab initio approach using a Green function method. Furthermore, we are able to calculate the electron and phonon temperature profile across the Fe/MgO/Fe MTJ by estimating the electron-phonon interaction in the Fe leads. Our results show that there is an electron-phonon temperature imbalance at the Fe-MgO interfaces. As a consequence, a revision of the interpretation of current experimental measurements may be necessary.

On/off switching of bit readout in bias-enhanced tunnel magneto-Seebeck effect.

Thermoelectric effects in magnetic tunnel junctions are promising to serve as the basis for logic devices or memories in a "green" information technology. However, up to now the readout contrast achieved with Seebeck effects was magnitudes smaller compared to the well-established tunnel magnetoresistance effect. Here, we resolve this problem by demonstrating that the tunnel magneto-Seebeck effect (TMS) in CoFeB/MgO/CoFeB tunnel junctions can be switched on to a logic "1" state and off to "0" by simply changing the magnetic state of the CoFeB electrodes. This new functionality is achieved by combining a thermal gradient and an electric field. Our results show that the signal crosses zero and can be adjusted by tuning a bias voltage that is applied between the electrodes of the junction; hence, the name of the effect is bias-enhanced tunnel magneto-Seebeck effect (bTMS). Via the spin- and energy-dependent transmission of electrons in the junction, the bTMS effect can be configured using the bias voltage with much higher control than the tunnel magnetoresistance and even completely suppressed for only one magnetic configuration. Moreover, our measurements are a step towards the experimental realization of high TMS ratios without additional bias voltage, which are predicted for specific Co-Fe compositions.

Implementation of non-equilibrium vertex corrections in KKR: transport through disordered layers.

The theoretical description of modern nanoelectronic devices requires a quantum mechanical treatment and often involves disorder, e.g. from alloys. Therefore, the ab initio theory of transport using non-equilibrium Green's functions is extended to the case of disorder described by the coherent potential approximation. This requires the calculation of non-equilibrium vertex corrections. We implement the vertex corrections in a Korringa-Kohn-Rostoker multiple scattering scheme. In order to verify our implementation and to demonstrate the accuracy and applicability we investigate a system of an iron-cobalt alloy layer embedded in copper. The results obtained with the coherent potential approximation are compared to supercell calculations. It turns out that vertex corrections play an important role for this system.

Seebeck effect in magnetic tunnel junctions.

Creating temperature gradients in magnetic nanostructures has resulted in a new research direction, that is, the combination of magneto- and thermoelectric effects. Here, we demonstrate the observation of one important effect of this class: the magneto-Seebeck effect. It is observed when a magnetic configuration changes the charge-based Seebeck coefficient. In particular, the Seebeck coefficient changes during the transition from a parallel to an antiparallel magnetic configuration in a tunnel junction. In this respect, it is the analogue to the tunnelling magnetoresistance. The Seebeck coefficients in parallel and antiparallel configurations are of the order of the voltages known from the charge-Seebeck effect. The size and sign of the effect can be controlled by the composition of the electrodes' atomic layers adjacent to the barrier and the temperature. The geometric centre of the electronic density of states relative to the Fermi level determines the size of the Seebeck effect. Experimentally, we realized 8.8% magneto-Seebeck effect, which results from a voltage change of about -8.7 µV K⁻¹ from the antiparallel to the parallel direction close to the predicted value of -12.1 µV K⁻¹. In contrast to the spin-Seebeck effect, it can be measured as a voltage change directly without conversion of a spin current.