Issue 30, 2014

Donor and acceptor impurity-driven switching of magnetic ordering in MnSb2−xSnxSe4

Abstract

The ability to manipulate the electronic structure of the low-dimensional magnetic semiconductor MnSb2Se4via isomorphic Sn/Sb substitutions enables independent investigation of the interactions of free carriers with localized magnetic moments and their effects on the predominant magnetic ordering in the p-type MnSb2−xSnxSe4 (0 ≤ x ≤ 0.25) semiconductors. We find a large increase in the electrical resistivity and thermopower with increasing Sn content suggesting a surprising decrease in the overall hole density. X-ray photoelectron spectroscopy reveals that Sn atoms enter the structure in the 2+ oxidation state, whereas a fraction of the remaining Sb3+ partially oxidizes to Sb5+ to maintain the electroneutrality of the compound. Therefore, we attribute the drop in the hole density to electron–hole compensation processes. Interestingly, magnetic susceptibility data reveal a remarkable switching of the dominant magnetic interaction from antiferromagnetism (AFM) (x = 0) to ferromagnetism (FM) with Tc ∼ 56 K for 0.05 ≤ x ≤ 0.15 samples and a reversal to AFM ordering for x > 0.15. The Sn-dependent FM interaction in MnSb2−xSnxSe4 is rationalized within the context of the formation of overlapping bound magnetic polarons (BMPs) through the interactions between the added electrons/holes and localized moments of Mn2+ magnetic ions.

Graphical abstract: Donor and acceptor impurity-driven switching of magnetic ordering in MnSb2−xSnxSe4

Article information

Article type
Paper
Submitted
02 Apr 2014
Accepted
14 May 2014
First published
16 May 2014

J. Mater. Chem. C, 2014,2, 6199-6210

Author version available

Donor and acceptor impurity-driven switching of magnetic ordering in MnSb2−xSnxSe4

H. Djieutedjeu, X. Zhou, H. Chi, N. Haldolaarachchige, K. G. S. Ranmohotti, C. Uher, D. Young and P. F. P. Poudeu, J. Mater. Chem. C, 2014, 2, 6199 DOI: 10.1039/C4TC00672K

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