Cation ordering, ferrimagnetism and ferroelectric relaxor behavior in Pb(Fe1\u2212xScx)2\u22153W1\u22153O3 solid solutions

Sergey A Ivanov,Samrand Shafeie,Per Nordblad,Alexandr A Bush,Duo Wang,Premysl Beran,Biplab Sanyal,Olle Eriksson,Roland Tellgren,Martin Sahlberg,Yaroslav Kvashnin,Tapati Sarkar,Roland Mathieu

doi:10.1140/epjb/e2019-100149-9

Sergey A Ivanov, Samrand Shafeie + Show 11 more

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https://doi.org/10.1140/epjb/e2019-100149-9

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Abstract

Ceramic samples of the multiferroic perovskite Pb(Fe1−xScx)2∕3W1∕3O3 with 0 ≤ x ≤ 0.4 have been synthesized using a conventional solid-state reaction method, and investigated experimentally and theoretically using first-principle calculations. Rietveld analyses of joint synchrotron X-ray and neutron diffraction patterns show the formation of a pure crystalline phase with cubic (Fm3̅m) structure with partial ordering in the B-sites. The replacement of Fe by Sc leads to the increase of the cation order between the B′ and B′′ sites. As the non-magnetic Sc3+ ions replace the magnetic Fe3+ cations, the antiferromagnetic state of PbFe2∕3W1∕3O3 is turned into a ferrimagnetic state reflecting the different magnitude of the magnetic moments on the B′ and B′′ sites. The materials remain ferroelectric relaxors with increasing Sc content. Results from experiments on annealed and quenched samples show that the cooling rate after high temperature annealing controls the degree of cationic order in Pb(Fe1−xScx)2∕3W1∕3O3 and possibly also in the undoped PbFe2∕3W1∕3O3.Graphical abstract

Highlights

The search for new multiferroic (MF) materials is driven by the hope to find materials that can be used for the transformation of a magnetic signal to an electric response, and vice versa [1,2,3]
After multiple grinding and heating cycles, the X-ray powder diffraction (XRPD) patterns collected from the PFSWO solid solutions were invariant, indicating that no further reaction was occurring
From inspection of these patterns, it was evident that there are three ranges in this composition series of compounds: single phase samples were obtained at each end of the compositional series and a two-phase region exists between them

Summary

Introduction

The search for new multiferroic (MF) materials is driven by the hope to find materials that can be used for the transformation of a magnetic signal to an electric response, and vice versa [1,2,3]. The most promising candidate materials for such applications are double perovskites [4,5,6]. PbFe2/3W1/3O3 (PFWO) belongs to the family of Pb-based 2:1 perovskites combining magnetically active Fe3+ cations with ferroelectrically active W6+ cations [7,8]. PFWO exhibits relaxor ferroelectric [9,10,11,12] behaviour between 150 K and 200 K and antiferromagnetic (AFM) order with a Neel temperature TN of approximately 350 K. An interesting peculiarity of the PFWO system in comparison with other MF perovskites is that the presence of Fe3+ with an occupancy of 2/3 on the B-octahedral sites of the perovskite cells leads to one of the highest magnetic ordering temperature in double perovskites [5].

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