Two-channel thermal transport and scattering channel of high-temperature phase SnSe using temperature-dependent effective potential

To resolve the imaginary phonon frequency of high-temperature phase SnSe (853 K) caused by ground-state theory, the temperature-dependent effective potential (TDEP) method is used to evaluate the temperature-dependent interatomic force constants (IFCs). Based on the Boltzmann transport equation, both two-channel transport and scattering channel are studied using the temperature-dependent IFCs. Considering three-phonon and four-phonon scattering, the particle-like thermal conductivity along the xx axis, yy axis, and zz axis is 0.66, 0.34, and 0.61 W/mK, respectively. For glass-like thermal conductivity, the value along the xx axis, yy axis, zz axis are 0.0777, 0.0316, and 0.0791 W/mK, respectively. For the three-phonon scattering channel, the scattering channels of X + O/A→O and X→O+O/A play a major role. For four-phonon scattering channel, the major scattering channels are X + O+A→O, X + A+A→O, X + O-O/A→A, X + A-O→A, X-O/A-O/A→O, X-O-A→A. By utilizing the crystal orbital Hamilton population (COHP) analysis, the low lattice thermal conductivity is attributed to the weak chemical bonds from anti-bonding orbitals between Se4p and Sn5s states. This work provides new insight into the physical mechanisms for thermal transport of high-temperature phase SnSe with strong anharmonic effects. [Display omitted] •The imaginary phonon frequency caused by the ground-state within conventional density-functional theory is resolved.•The optical/acoustic branch dominates the particle-like/glass-like thermal conductivity.•For the three-phonon scattering channel, the scattering channels of X+O/A→O and X→O+O/A play a major role..•The major scattering channels of four phonon are X+O+A→O, X+A+A→O, X+O-O/A→A, X+A-O→A, X-O/A-O/A→O, X-O-A→A.•The antibonding orbitals between Se4p and Sn5s leads to the low lattice thermal conductivity of SnSe.