Effect of small cation occupancy and anomalous Griffiths phase disorder in nonstoichiometric magnetic perovskites
JOURNAL OF ALLOYS AND COMPOUNDS(2022)
摘要
The structural, magnetic, magnetocaloric and Griffiths phase (GP) disorder of non-stoichiometric perovskite manganites La0.8-xSr0.2-yMn1+x+yO3 are reported here. Determination of valence states and structural phases evidenced that the smaller cations Mn2+ and Mn3+ will not occupy the A-site of a perovskite under atmospheric synthesis conditions. The same analysis also supports that the vacancy in the A-site of a perovskite induces a similar vacancy in the B-site. The La3+ and Sr2+ cation substitutions in the A-site with vacancy influences the magnetic phase transition temperature (TC) inversely, which is explained in terms of the electronic bandwidth change. An anomalous non-linear change of the GP has been observed in the Sr substituted compounds. The agglomeration of Mn3+-Mn4+ pairs (denoted as dimerons), into small ferromagnetic clusters, has been identified as the reason for the occurrence of the GP. A threshold limit of the dimeron formation explains the observed non-linear behaviour of the GP formation. The Sr-substituted compounds show a relatively large value of isothermal entropy change (maximum 3.27 J/kgK at mu H-0 = 2T) owing to its sharp magnetic transition, while the broad change of magnetization in the La-substituted compound enhances the relative cooling power (maximum 98 J/kg at mu H-0 = 2T). (C) 2021 The Author(s). Published by Elsevier B.V.
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关键词
Manganites,Magnetocaloric effect,Griffiths phase,Rutherford backscattering spectrometry,X-ray photoelectron spectroscopy,Nonstoichiometric perovskites
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