Phonon thermal transport in ferroelectric α-In2Se3 via first-principles calculations.

Two-dimensional (2D) ferroelectrics are promising candidates in the field of microelectronics due to their unique properties such as excellent photoelectric responsiveness. However, the thermal properties of 2D ferroelectrics are less investigated. Here, the thickness dependent thermal conductivity in ferroelectric α-In2Se3 is systematically investigated by the first-principles method combined with the phonon Boltzmann transport equation. On this basis, the strain and oxidation effects on the thermal conductivity of monolayer α-In2Se3 is further studied. The calculation results show that the thermal conductivity has a significant reduction with decreasing film thickness or increasing tensile strain, and the anharmonic phonon-phonon scattering rate is the intrinsic mechanism for the reduction in thermal conductivity. On the other hand, the replacement of Se atoms by O atoms can achieve a bidirectional and wide-range (12×) tuning of thermal conductivity. The increase in specific heat and phonon group velocity is responsible for the thermal conductivity enhancement at high doping levels while that in phonon-phonon scattering rate is responsible for the thermal conductivity reduction at low doping levels. In all cases, acoustic phonons dominate the in-plane thermal transport behavior. These findings broaden our understanding of phonon transport and its control in ferroelectric semiconductor α-In2Se3.