Prediction of Low-Thermal-Conductivity Compounds with First-Principles Anharmonic Lattice-Dynamics Calculations and Bayesian Optimization.

Compounds of low lattice thermal conductivity (LTC) are essential for seeking thermoelectric materials with high conversion efficiency. Some strategies have been used to decrease LTC. However, such trials have yielded successes only within a limited exploration space. Here, we report the virtual screening of a library containing 54,779 compounds. Our strategy is to search the library through Bayesian optimization using for the initial data the LTC obtained from first-principles anharmonic lattice-dynamics calculations for a set of 101 compounds. We discovered 221 materials with very low LTC. Two of them even have an electronic band gap <1 eV, which makes them exceptional candidates for thermoelectric applications. In addition to those newly discovered thermoelectric materials, the present strategy is believed to be powerful for many other applications in which the chemistry of materials is required to be optimized.

Direct solution to the linearized phonon Boltzmann equation.

The frequency dependent phonon Boltzmann equation is transformed to an integral equation over the irreducible part of the Brillouin zone. Simultaneous diagonalization of the collision kernel of that equation and a symmetry crystal class operator allow us to obtain a spectral representation of the lattice thermal conductivity valid at finite frequency. Combining this approach with density functional calculations, an ab initio dynamical thermal conductivity is obtained for the first time. The static thermal conductivity is also obtained as a particular case. The method is applied to C, Si, and Mg2Si and excellent agreement is obtained with the available static thermal conductivity measurements.

Implementation strategies in phonopy and phono3py.

Scientific simulation codes are public property sustained by the community. Modern technology allows anyone to join scientific software projects, from anywhere, remotely via the internet. The phonopy and phono3py codes are widely used open-source phonon calculation codes. This review describes a collection of computational methods and techniques implemented in these codes and shows their implementation strategies as a whole, aiming to be useful for the community. Some of the techniques presented here are not limited to phonon calculations and may therefore be useful in other areas of condensed matter physics.

Ab initio phonon properties of half-Heusler NiTiSn, NiZrSn and NiHfSn.

A theoretical investigation of phonon properties from first-principles calculations is carried out for the half-Heusler compounds NiXSn, [Formula: see text], Zr and Hf. The crystal structures are optimised via ab initio calculations within the framework of density functional theory. The phonon properties are retrieved from harmonic and anharmonic interatomic force constants calculations using the finite size displacements method and many-body perturbation theory. A solution to the linearized phonon Boltzmann transport equation is then used to compute the ab initio thermal conductivities. For X = Ti, Zr and Hf, we found 15.4, 13.3 and 15.8 W m(-1) K(-1) at 300 K, respectively. Thanks to a spectral analysis of the velocities and lifetimes we were able appreciate the differences in the thermal conductivities between the three compounds under study. Our results provide insights to understand the behaviour of the thermal conductivity and therefore to improve the thermoelectric figure of merit for such materials.

Giant spin-dependent thermoelectric effect in magnetic tunnel junctions.

Thermoelectric effects in magnetic nanostructures and the so-called spin caloritronics are attracting much interest. Indeed it provides a new way to control and manipulate spin currents, which are key elements of spin-based electronics. Here we report on a giant magnetothermoelectric effect in a magnetic tunnel junction. The thermovoltage in this geometry can reach 1 mV. Moreover a magnetothermovoltage effect could be measured with ratio similar to the tunnel magnetoresistance ratio. The Seebeck coefficient can then be tuned by changing the relative magnetization orientation of the two magnetic layers in the tunnel junction. Therefore, our experiments extend the range of spintronic devices application to thermoelectricity and provide a crucial piece of information for understanding the physics of thermal spin transport.