Unveiling Phonon Contributions to Thermal Transport and the Failure of the Wiedemann-Franz Law in Ruthenium and Tungsten Thin Films

TL;DR

This study demonstrates that phonons significantly contribute to thermal transport in ruthenium and tungsten thin films, leading to deviations from the Wiedemann-Franz law and offering insights for improved nanoscale thermal management.

Contribution

It reveals the substantial phonon contributions to thermal conductivity in Ru and W films and links these findings to deviations from classical laws and microstructural insensitivity.

Findings

Phonons contribute 45% in Ru and 62% in W to total thermal conductivity.

Deviations from Wiedemann-Franz law indicate strong phonon involvement.

Phonon transport is insensitive to microstructural variations.

Abstract

Thermal transport in nanoscale interconnects is dominated by intricate electron-phonon interactions and microstructural influences. As copper faces limitations at the nanoscale, tungsten and ruthenium have emerged as promising alternatives due to their substantial phonon contributions to thermal conductivity. Metals with stronger phonon-mediated thermal transport are particularly advantageous in nanoscale architectures, where phonons are less sensitive to size effects than electrons. Here, we show that phonons play a comparable role to electrons in the thermal transport of ruthenium and tungsten thin films, evidenced by deviations from the classical Wiedemann-Franz law. Elevated Lorenz numbers-1.9 and 2.7 times the Sommerfeld value for ruthenium and tungsten, respectively-indicate phonon contributions of 45% and 62% to total thermal conductivity. Comparisons of in-plane thermal conductivity from steady-state thermoreflectance and electron relaxation times from infrared ellipsometry reveal that phonon-mediated transport is insensitive to microstructural variations and scaling. Ultrafast infrared pump-probe measurements show that ruthenium exhibits a higher electron-phonon coupling factor than tungsten, consistent with the differing contributions of carriers to thermal transport. Molecular dynamics simulations and spectral energy density analysis confirm substantial phonon-driven thermal transport and mode-dependent phonon lifetimes. These results offer insights into phonon-driven thermal transport and provide design principles for selecting interconnects with enhanced thermal management.