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Register a new userEvidence of a cluster spin-glass state in the B-site disordered perovskite SrTi0.5Mn0.5O3
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SrTi0.5Mn0.5O3 (STMO) is a chemically disordered perovskite having random distribution of Ti and Mn over 1b site. Striking discrepancies about the structural and magnetic properties of STMO demands detailed analysis which is addressed. To explore the magnetic ground state of STMO, static and dynamic magnetic properties were studied over a broad temperature range (2-300 K). The dc, ac magnetization show a cusp like peak at Tf ~ 14 K, which exhibits field and frequency dependence. The thermoremanent magnetization is characterized by using stretched exponential function and characteristic time suggests the existence of spin clusters. Also the other features observed in magnetic memory effect, muon spin resonance/rotation and neutron powder diffraction confirm the existence of cluster spin glass state in STMO, rather than the long range ordered ground state. Intriguingly, the observed spin relaxation can be attributed to the dilute magnetism due to non-magnetic doping at Mn-site and competing antiferromagnetic and ferromagnetic interactions resulting from the site disorder.
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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.
Famous for its spin-state puzzle, LaSrCoO$_4$ (Co$^{3+}$) is an intermediate between antiferromagnetic (AFM) La$_2$CoO$_4$ (Co$^{2+}$) and ferromagnetic (FM) Sr$_2$CoO$_4$ (Co$^{4+}$). The appearance of the Co$^{3+}$ valence state (not present in the end compounds) is intriguing because of the spin-state transitions associated with it. In this work, we report two magnetic transitions in LaSrCoO$_4$: (i) a transition at T $=$ T$_c$ $simeq$ 225 K, from the paramagnetic state to a state with an inhomogeneous long-range ferromagnetic (FM) order wherein finite FM clusters coexist with infinite FM matrix in the percolation sense, and (ii) the transition to the cluster spin glass (CSG) state at T $=$ T$_g$ $simeq$ 8 K. Finite FM clusters (which at low temperatures give rise to the cluster spin glass state) and infinite FM matrix are formed due to the spin-spin interactions brought about by the inhomogeneously distributed Co$^{3+}$ high spin (HS) and Co$^{3+}$ low spin (LS) ions. A firm support to the presence of an unconventional (inhomogeneous) ferromagnetic order comes from the anomalous values of the critical exponents $beta$, $gamma$ and $delta$ for the spontaneous magnetization, `zero-field magnetic susceptibility and the critical M - H isotherm, while the coexistence of HS Co$^{3+}$ and LS Co$^{3+}$ ions is confirmed by the results of the extended X-ray absorption fine structure spectroscopy.
The study of the ferrites YBaFe4-xGaxO7 shows that the substitution of Ga for Fe in YBaFe4O7 stabilizes the hexagonal symmetry for 0.40 < x < 0.70, at the expense of the cubic one. Using combined measurements of a. c. and d. c. magnetization, we establish that Ga substitution for Fe in YBaFe4O7 leads to an evolution from a geometrically frustrated spin glass (for x = 0) to a cationic disorder induced spin glass (x = 0.70). We also find an intermediate narrow range of doping where the samples are clearly phase separated having small ferrimagnetic clusters embedded in a spin glass matrix. The origin of the ferrimagnetic clusters lies in the change in symmetry of the samples from cubic to hexagonal (and a consequent lifting of the geometrical frustration) as a result of Ga doping. We also show the presence of exchange bias and domain wall pinning in these samples. The cause of both these effects can be traced back to the inherent phase separation present in the samples.
Birnessite compounds are stable across a wide range of compositions that produces a remarkable diversity in their physical, electrochemical and functional properties. These are hydrated analogues of the magnetically frustrated, mixed-valent manganese oxide structures, with general formula, NaxMnO2. Here we demonstrate that the direct hydration of layered rock-salt type a-NaMnO2, with the geometrically frustrated triangular lattice topology, yields the birnessite type oxide, Na0.36MnO2 0.2H2O, transforming its magnetic properties. This compound has a much-expanded interlayer spacing compared to its parent a-NaMnO2 compound. We show that while the parent a-NaMnO2 possesses a Neel temperature of 45 K as a result of broken symmetry in the Mn3+ sub-lattice, the hydrated derivative undergoes collective spin-freezing at 29 K within the Mn3+/Mn4+ sub-lattice. Scaling-law analysis of the frequency dispersion of the AC susceptibility, as well as the temperature-dependent, low-field DC magnetization confirm a cooperative spin-glass state of strongly interacting spins. This is supported by complementary spectroscopic analysis (HAADF-STEM, EDS, EELS) as well as by a structural investigation (high-resolution TEM, X-ray and neutron powder diffraction) that yield insights into the chemical and atomic structure modifications. We conclude that the spin-glass state in birnessite is driven by the spin-frustration imposed by the underlying triangular lattice topology that is further enhanced by the in-plane bond-disorder generated by the mixed-valent character of manganese in the layers.
In conventional exchange-bias system comprising of a bilayer film of ferromagnet (FM) and antiferromagnet (AFM), investigating the role of spin-disorder and spin-frustration inside the AFM and at the interface has been crucial in understanding the fundamental mechanism controlling the exchange-bias -- an effect that leads to a horizontal shift in the magnetization hysteresis response of the FM. Similarly, in the recently reported monolayer molecular exchange-bias effect requiring no AFM layer, probing magnetic-disorder at the FM/molecule interface or inside the FM layer can provide new insights into the origin of molecular exchange-bias and the associated physics. In this article, by cooling the Fe/metal-phthalocyanine devices in oscillating magnetic field, we demonstrate a characteristic temperature dependent response of exchange-bias shift and ferromagnet coercivity that is supportive of a spin-glass behavior. Here, the origin of spin-glass is attributed to the spin frustration created in the magnetic structure of the Fe layer, which was absent in our reference-Fe studies. These results highlight the strong influence of FM/molecule interface pi-d hybridization on the magnetic exchange interactions extending deeper into the FM layer.
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