First-principles quantitative prediction of the lattice thermal conductivity in random semiconductor alloys: the role of force-constant disorder

Abstract

The standard theoretical understanding of the lattice thermal conductivity, ${\kappa }_{\ell }$, of semiconductor alloys assumes that mass disorder is the most important source of phonon scattering. In contrast, we show that the hitherto neglected contribution of force-constant (IFC) disorder is essential to accurately predict the ${\kappa }_{\ell }$ of those polar compounds characterized by a complex atomic-scale structure. We have developed an \emph{ab initio} method based on special quasirandom structures and Green's functions, and including the role of IFC disorder, and applied it in order to calculate the ${\kappa }_{\ell }$ of $\mathrm{I}{\mathrm{n}}_{1-\mathrm{x}}\mathrm{G}{\mathrm{a}}_{\mathrm{x}}\mathrm{As}$ and $\mathrm{S}{\mathrm{i}}_{1-\mathrm{x}}\mathrm{G}{\mathrm{e}}_{\mathrm{x}}$ alloys. We show that, while for $\mathrm{S}{\mathrm{i}}_{1-\mathrm{x}}\mathrm{G}{\mathrm{e}}_{\mathrm{x}}$, phonon-alloy scattering is dominated by mass disorder, for $\mathrm{I}{\mathrm{n}}_{1-\mathrm{x}}\mathrm{G}{\mathrm{a}}_{\mathrm{x}}\mathrm{As}$, the inclusion of IFC disorder is fundamental to accurately reproduce the experimentally observed ${\kappa }_{\ell }$. As the presence of a complex atomic-scale structure is common to most III-V and II-VI random semiconductor alloys, we expect our method to be suitable for a wide class of materials.

References in corpus (6)

• almaBTE: a solver of the space-time dependent Boltzmann transport equation for phonons in structured materials
• Exceptionally strong phonon scattering by B substitution in cubic SiC
• Superdiffusive heat conduction in semiconductor alloys -- I. Theoretical foundations
• Cross-plane heat conduction in thin films with ab-initio phonon dispersions and scattering rates
• Unraveling the dominant phonon scattering mechanism in thermoelectric compound ZrNiSn
• Phonon transport unveils the prevalent point defects in GaN

Cited by in corpus (13)

• High intrinsic lattice thermal conductivity in monolayer MoSi${}_2$N${}_4$
• Machine Learning for Predicting Thermal Transport Properties of Solids
• Comparing the performance of LDA and GGA functionals in predicting the lattice thermal conductivity of semiconductor materials: the case of AlAs
• Excellent Thermoelectric Performances of Pressure Synthesized ZnSe2
• Thermoelectric transport trends in group 4 half-Heusler alloys
• Effect of local chemistry and structure on thermal transport in doped GaAs
• Perturbation theory and thermal transport in mass-disordered alloys: Insights from Green's function methods
• Success and breakdown of the T-matrix approximation for phonon-disorder scattering
• Decorated dislocations against phonon propagation for thermal management
• Enhanced Thermoelectric Performance of Polycrystalline Si0.8Ge0.2 Alloys through the Addition of Nanoscale Porosity
• Uncertainty quantification in first-principles predictions of phonon properties and lattice thermal conductivity
• Discarded gems: Thermoelectric performance of materials with band gap emerging at the hybrid-functional level
• Structural effect on phonon attenuation in metallic liquids and glasses