Complex magnetic properties associated with competing local and itinerant magnetism in Pr2Co0.86Si2.88

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2021-06-24
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Kundu, Mily
Pakhira, Santanu
Choudhary, Renu
Paudyal, Durga
Lakshminarasimhan, N.
Avdeev, Maxim
Cottrell, Stephen
Adroja, Devashibhai
Ranganathan, R.
Mazumdar, Chandan
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Ames National LaboratoryElectrical and Computer Engineering
Abstract

Ternary intermetallic compound Pr2Co0.86Si2.88 has been synthesized in single phase and characterized by x-ray diffraction, scanning electron microscopy with energy dispersive x-ray spectroscopy (SEM-EDX) analysis, magnetization, heat capacity, neutron diffraction and muon spin rotation/relaxation (μSR) measurements. The polycrystalline compound was synthesized in single phase by introducing necessary vacancies in Co/Si sites. Magnetic, heat capacity, and zero-field neutron diffraction studies reveal that the system undergoes magnetic transition below ∼4 K. Neutron diffraction measurement further reveals that the magnetic ordering is antiferromagnetic in nature with an weak ordered moment. The high temperature magnetic phase has been attributed to glassy in nature consisting of ferromagnetic clusters of itinerant (3d) Co moments as evident by the development of internal field in zero-field μSR below 50 K. The density-functional theory (DFT) calculations suggest that the low temperature magnetic transition is associated with antiferromagnetic coupling between Pr 4f and Co 3d spins. Pr moments show spin fluctuation along with unconventional orbital moment quenching due to crystal field. The evolution of the symmetry and the crystalline electric field environment of Pr-ions are also studied and compared theoretically between the elemental Pr and when it is coupled with other elements such as Co. The localized moment of Pr 4f and itinerant moment of Co 3d compete with each other below ∼20 K resulting in an unusual temperature dependence of magnetic coercivity in the system.

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