Thermoelectric calculations of ring-shaped bands in two-dimensional Bi$_2$Te$_3$, Bi$_2$Se$_3$ and Sb$_2$Te$_3$: a comparison of simple scattering approximations

TL;DR

This study uses density functional theory to compare simple scattering approximations in thermoelectric calculations of 2D Bi$_2$Te$_3$, Bi$_2$Se$_3$, and Sb$_2$Te$_3$, highlighting the importance of the DOS scattering model for accurate performance predictions.

Contribution

It introduces a detailed comparison of scattering models, emphasizing the effectiveness of the DOS scattering approximation in predicting thermoelectric properties of 2D materials with ring-shaped bands.

Findings

Single quintuple-layer materials have two ring-shaped valence band maxima enhancing power factors.

The DOS scattering model predicts additional thermoelectric benefits from a ring-shaped minimum.

Double quintuple-layer materials show worse thermoelectric performance due to altered dispersions.

Abstract

Materials with ring-shaped electronic bands are promising thermoelectric candidates, since their unusual dispersion shape is predicted to give large power factors. While previous calculations of these materials have relied on the assumption of a constant mean-free-path or relaxation time, recent first-principles modeling of electron-phonon scattering suggests that the scattering rates may be better approximated by the electron density-of-states (so-called DOS scattering model). In this work, we use density functional theory to investigate single and double quintuple-layer Bi$_2$Te$_3$, Bi$_2$Se$_3$ and Sb$_2$Te$_3$, with a focus on understanding how the three aforementioned scattering approximations impact thermoelectric performance -- emphasis is placed on the DOS scattering model. The single quintuple-layer materials possess two ring-shaped valence band maxima that provide an abrupt increase in conducting channels, which benefits the power factor. Additionally, below the band edge a ring-shaped minimum, located between the two maxima, is found to further enhance the thermoelectric performance but only with the DOS scattering model. This comes from a sharp drop in the DOS, and thus scattering, just below the ring-shaped minimum. An analytic octic dispersion model is introduced and shown to qualitatively capture the observed features. The double quintuple-layer materials display notably worse thermoelectric properties, since their dispersions are significantly modified compared to the single quintuple-layer case. The benefits of ring-shaped bands are sensitive to the alignment of the two ring maxima and to the degree of ring anisotropy. Overall, single quintuple-layer Bi$_2$Te$_3$ and Bi$_2$Se$_3$ are most promising, with the DOS scattering model giving the highest power factors.