Design of $n$- and $p$-type oxide thermoelectrics in LaNiO${}_3$/SrTiO${}_3(001)$ superlattices exploiting interface polarity

Abstract

We investigate the structural, electronic, transport, and thermoelectric properties of LaNiO${}_3$/SrTiO${}_3(001)$ superlattices containing either exclusively $n$- or $p$-type interfaces or coupled interfaces of opposite polarity by using density functional theory calculations with an on-site Coulomb repulsion term. The results show that significant octahedral tilts are induced in the SrTiO${}_3$ part of the superlattice. Moreover, the La-Sr distances and Ni-O out-of-plane bond lengths at the interfaces exhibit a distinct variation by about $7\%$ with the sign of the electrostatic doping. In contrast to the much studied LaAlO${}_3$/SrTiO${}_3$ system, the charge mismatch at the interfaces is exclusively accommodated within the LaNiO${}_3$ layers, whereas the interface polarity leads to a band offset and to the formation of an electric field within the coupled superlattice. Features of the electronic structure indicate an orbital-selective quantization of quantum well states. The potential- and confinement-induced multiband splitting results in complex cylindrical Fermi surfaces with a tendency towards nesting that depends on the interface polarity. The analysis of the thermoelectric response reveals a particularly large positive Seebeck coefficient ($135\mu$V/K) and a high figure of merit ($0.35$) for room-temperature cross-plane transport in the $p$-type superlattice that is attributed to the participation of the SrTiO${}_3$ valence band. Superlattices with either $n$- or $p$-type interfaces show cross-plane Seebeck coefficients of opposite sign and thus emerge as a platform to construct an oxide-based thermoelectric generator with structurally and electronically compatible $n$- and $p$-type oxide thermoelectrics.

11 pages, 9 figures

References in corpus (9)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• BoltzTraP. A code for calculating band-structure dependent quantities
• Avoiding the polarization catastrophe in LaAlO3 overlayers on SrTiO3(001) through a polar distortion
• Fermi surfaces, electron-hole asymmetry and correlation kink in a three-dimensional Fermi liquid LaNiO${}_3$
• Giant Oscillating Thermopower at Oxide Interfaces
• Polar catastrophe in ultra-thin limit: A case of rare-earth perovskite LaNiO3
• Confinement-induced metal-to-insulator transition in strained LaNiO${}_3$/LaAlO${}_3$ superlattices
• Ordering and multiple phase transitions in ultra-thin nickelate superlattices
• Latent Instabilities in Metallic LaNiO3 Films by Strain Control of Fermi-Surface Topology