Phonons in random alloys: the itinerant coherent-potential approximation

We have investigated the effect of mass contrast on alloy phonon scattering in mass-substituted Lennard-Jones crystals. By calculating the mass-difference phonon scattering rate using a modal analysis method based on molecular dynamics, we have identified the applicability and limits of the widely-used mass-difference perturbation model in terms of magnitude and sign of the mass difference. The result of a phonon -mode-dependent analysis reveals that the critical phonon frequ...

By applying an unrestriced Hartree-Fock approximation and a Random Phase approximation to multiband Peierls-Hubbard Hamiltonians, we determine the phonon mode structure in models of transition metal oxides in the presence of intrinsic nanoscale inhomogeneities induced by hole doping. We identify low frequency $local$ vibrational modes pinned to the interface between regions of distinct electronic structure and separated in frequency from the band of extended phonons. A major ...

The random-phase approximation (RPA) as an approach for computing the electronic correlation energy is reviewed. After a brief account of its basic concept and historical development, the paper is devoted to the theoretical formulations of RPA, and its applications to realistic systems. With several illustrating applications, we discuss the implications of RPA for computational chemistry and materials science. The computational cost of RPA is also addressed which is critical ...

We present an accurate and efficient formulation for the calculation of phonons in real-space Kohn-Sham density functional theory. Specifically, employing a local exchange-correlation functional, norm-conserving pseudopotential in the Kleinman-Bylander representation, and local form for the electrostatics, we derive expressions for the dynamical matrix and associated Sternheimer equation that are particularly amenable to the real-space finite-difference method, within the fra...

almaBTE is a software package that solves the space- and time-dependent Boltzmann transport equation for phonons, using only ab-initio calculated quantities as inputs. The program can predictively tackle phonon transport in bulk crystals and alloys, thin films, superlattices, and multiscale structures with size features in the nm-$\mu$m range. Among many other quantities, the program can output thermal conductances and effective thermal conductivities, space-resolved average ...

Understanding and quantifying the fundamental physical property of coherence of thermal excitations is a long-standing and general problem in physics. The conventional theory, i.e. the phonon gas model, fails to describe coherence and its impact on thermal transport. In this letter, we propose a general heat conduction formalism supported by theoretical arguments and direct atomic simulations, which takes into account both the conventional phonon gas model and the wave nature...

Interest in high entropy alloy thermoelectric materials is predicated on achieving ultralow lattice thermal conductivity $\kappa\sub{L}$ through large compositional disorder. However, here we show that for a given mechanism, such as mass contrast phonon scattering, $\kappa\sub{L}$ will be minimized along the binary alloy with the highest mass contrast, such that adding an intermediate-mass atom to increase atomic disorder can increase thermal conductivity. Only when each comp...

Thermal properties are of great interest in modern electronic devices and nanostructures. Calculating these properties is straightforward when the device is made from a pure material, but problems arise when alloys are used. Specifically, only approximate bandstructures can be computed for random alloys and most often the Virtual Crystal Approximation (VCA) is used. Unfolding methods [T. B. Boykin, N. Kharche, G. Klimeck, and M. Korkusinski, J. Phys.: Condens. Matt. 19, 03620...

The class of the Generalized Coherent Potential Approximations (GCPA) to the Density Functional Theory (DFT) is introduced within the Multiple Scattering Theory formalism for dealing with, ordered or disordered, metallic alloys. All GCPA theories are based on a common ansatz for the kinetic part of the Hohenberg-Kohn functional and each theory of the class is specified by an external model concerning the potential reconstruction. The GCPA density functional consists of margin...

As a fundamental physical quantity of thermal phonons, temporal coherence participates in a broad range of thermal and phononic processes, while a clear methodology for the measurement of phonon coherence is still lacking. In this Lettter, we derive a theoretical model for the experimental exploration of phonon coherence based on spectroscopy, which is then validated by comparison with Brillouin light scattering data and direct molecular dynamic simulations of confined modes ...