Author:
Ichibha Tom,Saritas Kayahan,Krogel Jaron T.,Luo Ye,Kent Paul R. C.,Reboredo Fernando A.
Abstract
AbstractThe properties of $$\hbox{LaMO}_3$$
LaMO
3
(M: 3d transition metal) perovskite crystals are significantly dependent on point defects, whether introduced accidentally or intentionally. The most studied defects in La-based perovskites are the oxygen vacancies and doping impurities on the La and M sites. Here, we identify that intrinsic antisite defects, the replacement of La by the transition metal, M, can be formed under M-rich and O-poor growth conditions, based on results of an accurate many-body ab initio approach. Our fixed-node diffusion Monte Carlo (FNDMC) calculations of $$\hbox{LaMO}_3$$
LaMO
3
($$\hbox{M} = \hbox{Mn}$$
M
=
Mn
, Fe, and Co) find that such antisite defects can have low formation energies and are magnetized. Complementary density functional theory (DFT)-based calculations show that Mn antisite defects in $$\hbox{LaMnO}_3$$
LaMnO
3
may cause the p-type electronic conductivity. These features could affect spintronics, redox catalysis, and other broad applications. Our bulk validation studies establish that FNDMC reproduces the antiferromagnetic state of $$\hbox{LaMnO}_3$$
LaMnO
3
, whereas DFT with PBE (Perdew–Burke–Ernzerhof), SCAN (strongly constrained and appropriately normed), and the LDA+U (local density approximation with Coulomb U) functionals all favor ferromagnetic states, at variance with experiment.
Funder
The US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division
Publisher
Springer Science and Business Media LLC
Cited by
1 articles.
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