B-site spin-state and anti-site disorder driven multiple-magnetic phases: Griffiths phase, re-entrant cluster glass and exchange bias in double perovskite Pr${}_2$CoFeO${}_6$

Abstract

We report the comprehensive experimental results identifying the magnetic spin ordering and the magnetization dynamics of a double perovskite Pr2CoFeO6 by employing the (dc and ac) magnetization, powder neutron diffraction (NPD) and X-ray magnetic circular dichroism (XMCD) techniques. X-ray diffraction and neutron diffraction studies revealed that Pr2CoFeO6 adopts a B-site disordered orthorhombic structure with space group Pnma. Additionally, ab initio band structure calculations performed on this system suggested an insulating anti-ferromagnetic (Fe-Fe) ground state. Magnetometry study showed the system to possess a spectrum of interesting magnetic phases including long range antiferromagnetic (canted) spin ordering (TN ~269 K), Griffiths phase, re-entrant cluster glass (RCG) (TG~ 34 K) and exchange bias. However, the NPD study divulged the exhibition of a long range G-type (below TN ~269 K) of spin ordering by Fe spins. Spin dynamics study by ac susceptibility technique confirmed the system possessing long range ordering at higher temperatureundergoes a RCG transition at ~34 K. Existence of Griffiths phase was confirmed by non-analytic field variation of magnetization and Heisenberg type temporal spin relaxation above long range ordering temperature TN ~269 K. The anti-site disorder related to the B-sites (Co/Fe) is found to be the main driving force forthe observed multiple magnetic phases. Furthermore, the electronic structure probed by the X-ray absorption spectroscopy (XAS) study suggested a nominal valance state of +3 for both of the B-site ions (Co/Fe) which in turn triggered the anti-site disorder in the system. Magnetic, XRD, NPD and XAS analysis yielded a low spin state (LS) for the Co3+ ions. The random non-magnetic dilution of magnetic Fe3+ (HS) ions by Co3+ (LS) ions essentially played a crucial role in manifesting the magnetic properties of the system.

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• Frustration, strain and phase co-existence in the mixed valent hexagonal iridate Ba${}_3$NaIr${}_2$O${}_9$
• Observation of sharp metamagnetic transition, Griffiths like phase and glassy nature in double perovskite Eu2CoMnO6
• Disorder-Induced Griffiths like Phase and Charge Localization in Sr2FeRuO6
• Coexistence of Griffiths phase and superparamagnetic-like behavior in La-doped antiferromagnetic CaMnO3