Beyond the Tamura model of phonon-isotope scattering

The Tamura model is a particular type of first Born approximation of the phonon-isotope scattering problem. The expression for the mode-resolved phonon-isotope scattering rates in this model, derived in 1983, is still widely used in ab initio transport calculations. While the original work emphasized its applicability to low-energy acoustic phonons only, nevertheless, it has also been applied to optical phonons in the field of phonon transport. The model has the salient feature of being a perturbation theory on top of a virtual-crystal background. As such, this approach does not correspond to the proper methodology for solving the phonon-substitution defect problem in the respective limit. Here we explore three avenues to go beyond the Tamura model and carry out calculations on a set of common materials to compare the different approaches. This work allows a systematic improvement of the treatment of phonon-isotope scattering in ab initio phonon transport while unifying it with the general phonon-substitution scattering problem.