# Phonon Confinement and Transport in Ultrathin Films

## TL;DR

This study investigates phonon-mediated thermal transport in ultrathin films using advanced lattice dynamics and molecular dynamics simulations, revealing size-dependent behaviors and confinement effects that challenge traditional models.

## Contribution

It introduces a two-dimensional lattice dynamics approach that accurately captures phonon confinement effects in ultrathin films, improving upon traditional three-dimensional models.

## Key findings

- Thermal conductivity decreases with film thickness down to 2-3 nm.
- Confinement effects emerge below 5-6 nm thickness.
- Bulk phonon properties with boundary scattering models fail at low thicknesses.

## Abstract

Thermal transport by phonons in films with thicknesses of less than 10 nm is investigated in a soft system (Lennard-Jones argon) and a stiff system (Tersoff silicon) using two-dimensional lattice dynamics calculations and the Boltzmann transport equation. This approach uses a unit cell that spans the film thickness, which removes approximations related to the finite cross-plane dimension required in typical three-dimensional-based approaches. Molecular dynamics simulations are performed to obtain finite-temperature structures for the lattice dynamics calculations and to predict thermal conductivity benchmarks. Thermal conductivity decreases with decreasing film thickness until the thickness reaches four unit cells (2.1 nm) for argon and three unit cells (1.6 nm) for silicon. With a further decrease in film thickness, thermal conductivity plateaus in argon while it increases in silicon. This unexpected behavior, which we identify as a signature of phonon confinement, is a result of an increased contribution from low-frequency phonons, whose density of states increases as the film thickness decreases. Phonon mode-level analysis suggests that confinement effects emerge below thicknesses of ten unit cells (5.3 nm) for argon and six unit cells (3.2 nm) for silicon. Thermal conductivity predictions based on the bulk phonon properties combined with a boundary scattering model do not capture the low thickness behavior. To match the two-dimensional lattice dynamics and molecular dynamics predictions for larger thicknesses, the three-dimensional lattice dynamics calculations require a finite specularity parameter that in some cases approaches unity. These findings point to the challenges associated with interpreting experimental thermal conductivity measurements of ultrathin silicon films, where surface roughness and a native oxide layer impact phonon transport.