Tensile strain and finite size modulation of low lattice thermal conductivity in monolayer TMDCs (HfSe2 and ZrS2) from first-principles: a comparative study

Abstract

With excellent physical and chemical properties, 2D TMDC materials have been widely used in engineering applications, but they inevitably suffer from the dual effects of strain and device size. As typical 2D TMDCs, HfSe₂ and ZrS₂ are reported to have excellent thermoelectric properties. Thermal transport properties have great significance for exerting the performance of materials, ensuring device lifetime and stable operation, but current research is not detailed enough. Here, first-principles combined with the phonon Boltzmann transport equation are used to study the phonon transport inside monolayer HfSe₂ and ZrS₂ under tensile strain and finite size, and explore the band structure properties. Our research shows that they have similar phonon dispersion curve structures, and the band gap of HfSe₂ increases monotonically with the increase of tensile strain, while the bandgap of ZrS₂ increases and then decreases with the increase of tensile strain. Thermal conductivity has obvious strain dependence: with the increase of tensile strain, the thermal conductivity of HfSe₂ gradually decreases, while that of ZrS₂ increases slightly, and then gradually decreases. Reducing the system size can limit the contribution of phonons with a long mean free path, significantly decreasing thermal conductivity through the controlling effect of tensile strain. The mode contribution of thermal conductivity is systematically investigated, and anharmonic properties including mode and frequency-level scattering rates, group velocity and Grüneisen parameters are used to explain the associated mechanism. Phonon scattering processes and channels in various cases are discussed in detail. Our research provides a detailed understanding of the phonon transport and electronic structural properties of low thermal conductivity monolayers of HfSe₂ and ZrS₂, and further completes the study of thermal transport of the two materials under strain and size tuning, which will provide a foundation for further popularization and application.