We investigate the evolution of the cross-plane thermal conductivity $\kappa$ of superlattices (SLs) as interfaces change from perfectly abrupt to totally intermixed, by using nonequilibrium molecular dynamics simulations in combination with the spectral heat current calculations. We highlight the role of surface-interdiffusion-driven intermixing by calculating the $\kappa$ of SLs with changing interface roughness, whose tuning allows for $\kappa$ values much lower than the “alloy limit” and the abrupt interface limit in same cases. The interplay between alloy and interface scattering in different frequency ranges provides a physical basis to predict a minimum of thermal conductivity. More specifically, we also explore how the interface roughness affects the thermal conductivities for SL materials with a broad span of atomic mass and bond strength. In particular, we find that (i) only when the “spacer” thickness of SLs increases up to a critical value, $\kappa$ of rough SLs can break the corresponding “alloy limit,” since SLs with different “spacer” thickness have different characteristic length of phonon transport, which is influenced by surface-interdiffusion-driven intermixing to different extend. (ii) Whether $\kappa$ changes monotonically with interface roughness strongly depends on the period length and intrinsic behavior of phonon transport for SL materials. Especially, for the SL with large period length, there exists an optimal interface roughness that can minimize the thermal conductivity. (iii) Surface-interdiffusion-driven intermixing is more effective in achieving a low $\kappa$ below the alloy limit for SL materials with large mass mismatch than with small one. (iv) It is possible for SL materials with large lattice mismatch (i.e., bond strength) to design an ideally abrupt interface structure with $\kappa$ much below the alloy limit. These results have clear implications for optimization of thermal transport for heat management and for the development of thermoelectric materials.

• Received 11 August 2017

DOI:https://doi.org/10.1103/PhysRevMaterials.2.015401