Thermopower enhancement from engineering the Na$_{0.7}$CoO$_2$ interacting fermiology via Fe doping

TL;DR

This study combines theory and experiments to show that Fe doping in Na$_{0.7}$CoO$_2$ enhances thermopower by modifying its Fermi surface and inducing effective hole doping, offering a new route to improve thermoelectric performance.

Contribution

It demonstrates that Fe doping in Na$_{0.7}$CoO$_2$ alters the Fermi surface and increases thermopower, providing a novel approach to engineer thermoelectric properties in correlated materials.

Findings

Fe doping increases Seebeck coefficient.

Doping induces multi-sheet interacting Fermi surface.

Effective hole doping shifts hole pockets to lower energy.

Abstract

The sodium cobaltate system Na$_{x}$CoO$_2$ is a prominent representant of strongly correlated materials with promising thermoelectric response. In a combined theoretical and experimental study we show that by doping the Co site of the compound at $x$=0.7 with iron, a further increase of the Seebeck coefficient is achieved. The Fe defects give rise to effective hole doping in the high-thermopower region of larger sodium content $x$. Originally filled hole pockets in the angular-resolved spectral function of the Fe-free material shift to low energy when introducing Fe, leading to a multi-sheet interacting Fermi surface. Because of the higher sensitivity of correlated materials to doping, introducing adequate substitutional defects is thus a promising route to manipulate their thermopower.