Tuning of the carrier localization, magnetic and thermoelectric properties in ultrathin (LaNiO$_{3-\delta}$)$_1$/(LaAlO$_{3}$)$_1$(001) superlattices by oxygen vacancies

TL;DR

This study uses advanced computational methods to show how oxygen vacancies can precisely tune the electronic, magnetic, and thermoelectric properties of ultrathin LaNiO3/LaAlO3 superlattices, revealing potential for tailored material functionalities.

Contribution

It introduces a detailed theoretical analysis of oxygen vacancy effects on ultrathin nickelate superlattices, highlighting new ways to control their properties for applications.

Findings

Oxygen vacancies induce charge-disproportionation and ferrimagnetism.

A robust n-type thermoelectric power factor is achieved at certain vacancy levels.

Pristine and vacancy-ordered superlattices are dynamically stable.

Abstract

Using a combination of density functional theory calculations with an on-site Coulomb repulsion term (DFT+$U$) and Boltzmann transport theory within the constant relaxation time approximation, we explore the effect of oxygen vacancies on the electronic, magnetic, and thermoelectric properties in ultrathin (LaNiO$_{3-\delta}$)$_1$/(LaAlO$_{3}$)$_1$(001) superlattices (SLs). For the pristine SL, an antiferromagnetic charge-disproportionated (AFM-CD) ($d^{8}${$\underline L$}$^{2}$)$_{S=0}$($d^{8}$)$_{S=1}$ phase is stabilized, irrespective of strain. At $\delta$ = 0.125 and 0.25, the localization of electrons released from the oxygen defects in the NiO$_{2}$ plane triggers a charge-disproportionation, leading to a ferrimagnetic insulator both at $a_{\mathrm{STO}}$ (tensile strain) and $a_{\mathrm{LSAO}}$ (compressive strain). At $\delta$ = 0.5, an insulating phase emerges with alternating stripes of Ni$^{2+}$ (high-spin) and Ni$^{2+}$ (low-spin) and oxygen vacancies ordered along the [110] direction (S-AFM), irrespective of strain. This results in a robust $n$-type in-plane power factor of 24~$\mu$W/K$^2$ cm at $a_{\mathrm{STO}}$ and 14~$\mu$W/K$^2$ cm at $a_{\mathrm{LSAO}}$ at 300~K (assuming relaxation time $\tau = 4$~fs). Additionally, the pristine and $\delta$ = 0.5 SLs are shown to be dynamically stable. This demonstrates the fine tunability of electronic, magnetic, and thermoelectric properties of ultrathin nickelate superlattices by oxygen vacancies.