Tuning the carrier localization, magnetic and thermoelectric properties of ultrathin (LaNiO 3−δ ) 1/(LaAlO 3 )1 (001) superlattices by oxygen vacancies

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 (LaNiO3<−δ)1/(LaAlO3)1(001) superlattices (SLs). For the pristine SL (δ=0), an antiferromagnetic charge-disproportionated (AFM-CD) (d8L––2)S=0(d8)S=1 phase is stabilized, irrespective of strain. At δ=0.125 and 0.25, the localization of electrons released from the oxygen defects in the NiO2 plane triggers a charge-disproportionation, leading to a ferrimagnetic insulator both at aSrTiO3 (tensile strain) and aLaSrAlO4 (compressive strain). At δ=0.5, an insulating phase emerges with alternating stripes of Ni2+ (high-spin) and Ni2+ (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 24µW/K2 cm at aSTO and 14µW/K2 cm at aLSAO at 300 K (assuming relaxation time τ=4 fs). Additionally, the pristine and δ = 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.

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