Potential thermoelectric materials $\mathrm{CsM}{\mathrm{I}}_3$ (M=Sn and Pb) in perovskite structures from the first-principles calculations

Abstract

The thermoelectric properties of halide perovskites $\mathrm{CsM}{\mathrm{I}}_3$ (M=Sn and Pb) are investigated from a combination of first-principles calculations and semiclassical Boltzmann transport theory by considering both the electron and phonon transport. The electronic part is performed using a modified Becke and Johnson (mBJ) exchange potential, including spin-orbit coupling (SOC), while the phonon part is computed using generalized gradient approximation (GGA). It is found that SOC has remarkable detrimental effect on n-type power factor, while has a negligible influence in p-type doping, which can be explained by considering SOC effect on conduction and valence bands. Calculated results show exceptionally low lattice thermal conductivities in $\mathrm{CsSn}{\mathrm{I}}_3$ and $\mathrm{CsPb}{\mathrm{I}}_3$, and the corresponding room-temperature lattice thermal conductivity is 0.54 $\mathrm{W}{\mathrm{m}}^{-1}{\mathrm{K}}^{-1}$ and 0.25 $\mathrm{W}{\mathrm{m}}^{-1}{\mathrm{K}}^{-1}$. At 1000 K, the maximal figure of merit $ZT$ is up to 0.63 and 0.64 for $\mathrm{CsSn}{\mathrm{I}}_3$ and $\mathrm{CsPb}{\mathrm{I}}_3$ with scattering time $\tau$=$10^{-14}$ s, and the peak $ZT$ is 0.49 and 0.41 with $\tau$=$10^{-15}$ s. These results make us believe that $\mathrm{CsM}{\mathrm{I}}_3$ (M=Sn and Pb) in perovskite structures may be potential thermoelectric materials.

6 pages, 6 figures