Growth monitoring with sub-monolayer sensitivity via real time thermal conductance measurements

TL;DR

This paper presents a novel method using real-time thermal conductance measurements to monitor early film growth microstructure with sub-monolayer sensitivity, providing insights into cluster formation and film percolation.

Contribution

The work introduces a silicon nitride membrane sensor with high resolution for in-situ monitoring of film microstructure during growth, utilizing the 3ω method for precise thermal conductance measurements.

Findings

Thermal conductance decreases during initial nanocluster formation.

Conductance reaches a minimum at the percolation threshold.

Post-percolation, conductance increases linearly with film thickness.

Abstract

Growth monitoring during the early stages of film formation is of prime importance to understand the growth process, the microstructure and thus the overall layer properties. In this work, we demonstrate that phonons can be used as sensitive probes to monitor real time evolution of film microstructure during growth, from incipient clustering to continuous film formation. For that purpose, a silicon nitride membrane-based sensor has been fabricated to measure in-plane thermal conductivity of thin film samples. Operating with the 3{\omega}-V\"olklein method at low frequencies, the sensor shows an exceptional resolution down to {\Delta}({\kappa}*t)=0.065 nm*W/(m*K), enabling accurate measurements. Validation of the sensor performance is done with organic and metallic thin films. In both cases, at early stages of growth, we observe an initial reduction of the effective thermal conductance of the supporting amorphous membrane, K, related with the surface phonon scattering enhanced by the incipient nanoclusters formation. As clusters develop, K reaches a minimum at the percolation threshold. Subsequent island percolation produces a sharp increase of the conductance and once the surface coverage is completed K increases linearly with thickness The thermal conductivity of the deposited films is obtained from the variation of K with thickness.