Thermal conductivity of amorphous and crystalline GeTe thin film at high temperature: Experimental and theoretical study

TL;DR

This study combines experimental measurements and theoretical modeling to analyze the high-temperature thermal conductivity of amorphous and crystalline GeTe thin films, crucial for phase change memory device performance.

Contribution

It provides a comprehensive experimental and theoretical analysis of GeTe's thermal conductivity at high temperatures, including the effects of phase change and vacancy contributions.

Findings

Experimental thermal conductivity data for amorphous and crystalline GeTe.

Theoretical models accurately predict trends in thermal conductivity.

Identification of Umklapp scattering as the dominant phonon process.

Abstract

Thermal transport properties bear a pivotal role in influencing the performance of phase change memory (PCM) devices, in which the PCM operation involves fast and reversible phase change between amorphous and crystalline phases. In this paper, we present a systematic experimental and theoretical study on the thermal conductivity of GeTe at high temperatures involving fast change from amorphous to crystalline phase upon heating. Modulated photothermal radiometry (MPTR) is used to experimentally determine thermal conductivity of GeTe at high temperatures in both amorphous and crystalline phases. Thermal boundary resistances are accurately taken into account for experimental consideration. To develop a concrete understanding of the underlying physical mechanism, rigorous and in-depth theoretical exercises are carried out. For this, first-principles density functional methods and linearized Boltzmann transport equations (LBTE) are employed using both direct and relaxation time based approach (RTA) and compared with that of the phenomenological Slack model. The amorphous phase experimental data has been described using the minimal thermal conductivity model with sufficient precision. The theoretical estimation involving direct solution and RTA method are found to retrieve well the trend of the experimental thermal conductivity for crystalline GeTe at high temperatures despite being slightly overestimated and underestimated, respectively, compared to the experimental data. A rough estimate of vacancy contribution has been found to modify the direct solution in such a way that it agrees excellently with the experiment. Umklapp scattering has been determined as the significant phonon-phonon scattering process. Umklapp scattering parameter has been identified for GeTe for the whole temperature range which can uniquely determine and compare Umklapp scattering processes for different materials