Search results for: Buyisiwe Sondezi

Authors: Sibusiso Nqayi, Buyisiwe Sondezi

Abstract:

This investigation concentrates on the complex interrelations of intermediate valence states of cerium (Ce³⁺/Ce⁴⁺) and their respective contributions to distinctive magnetic phenomena, including antiferromagnetic (AFM) and ferromagnetic (FM) orderings, in addition to Griffith's phase. The Sm₂MnCeO₆+δ (SMCO) ceramic was prepared using the high-temperature solid-state method and crystallized in a cubic crystal structure with an Ia3d space group, possessing a uniform distribution of constituent elements. Magnetic susceptibility measurements reveal a Néel temperature (TN) of 13.8 K, indicating AFM behaviour, alongside evidence of Griffith's phase (GP) dynamics, 46.2 ≤T≤139.1 K. This phase follows a ferromagnetic (FM) ordering at Curie temperature (TC) of 43.7 K, which is an indication of the presence of short-range ordering of spins. The simultaneous presence of various oxidation states and their influence on both magnetic and structural characteristics positions SMCO as a versatile material proficient in functioning under elevated temperature conditions. This research paves the way for innovative applications of magnetic ceramics in the realms of catalysis, solid oxide fuel cells (SOFCs), and spintronics devices.

Keywords: Sm₂MnCeO₆+δ, ceramics, Néel temperature, Curie temperature, Griffith's phase

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Authors: S. Nqayi, B. Sondezi

Abstract:

A rare-earth-based Sm₂MnRuO₆₊δ (SMRO) double perovskite was prepared using a high-temperature solid-state reaction. The structural, morphological, chemical, thermodynamic, and magnetic properties were measured with X-ray diffraction (XRD), energy dispersive spectroscopy (EDS), X-ray photoemission spectroscopy (XPS), and vibrating sample magnetometer (VSM), respectively. The XRD revealed a tetragonal structure belonging to the I4/mmm space group, number 139, with linear Mn−O−Ru bonds. Replacing the well-studied alkaline earth metal with a rare-earth element increased the Mn-O bond length difference between the shorter equatorial (Mn-Oab) and the axial (Mn-Oc) bonds by approximately 6.3%. The elemental composition showed an O-rich double perovskite with a Ru deficit, which encourages the formation of a Ru⁶⁺ (d²) state. XPS spectra of Sm-3d, Ru-3d, and Mn-2p revealed the coexistence of a double oxidation state for each cation; Sm²⁺, Sm³⁺, Ru³⁺, Ru⁶⁺, Mn²⁺ , and Mn³⁺, in varying proportions. Entropy studies showed drastic ordering of spins at low temperatures (up to 12.4 K), whilst increasing temperatures above this point resulted in a drastic increase of disorder of the spins (up to 43.26 K), beyond which a constant slope of entropy is observed. Magnetic measurements revealed two magnetic ground states at TN = 12.4 K and TC = 43.3 K ordering antiferromagnetically (AFM) and ferromagnetically (FM), respectively. Kneller fit further showed that the materials become completely paramagnetic at TB = 88.1 K, (the blocking temperature). The existence of ferromagnetic (FM) super-exchange coupling in this work originating from Mn³⁺ (t³₂𝓰e¹𝓰)−O−Ru³⁺ (t⁵₂𝓰e⁰𝓰) and Mn²⁺ (t³₂𝓰e²𝓰−O−Ru⁶⁺ (t²₂𝓰e⁰𝓰) which plays an important role in suppressing the Mn/Ru−O−Mn/Ru antiferromagnetic (AFM) interactions.

Keywords: solid-state reaction, super-exchange coupling, ferromagnetic, Kneller’s law, entropy

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