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Register a new userB-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$_6$
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Sandip Chatterjee Professor
Publication date
2018
fields
Physics
and research's language is
English
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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.
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The structural and magnetic properties of double perovskiteTb2CoMnO6 have been investigated. Electronic structure analysis by XPS study reveals the presence of mixed oxidation state (Mn4+/Mn3+ and Co2+/Co3+) of B-site ions. The dc and ac magnetization measurements reveal different interesting phases such as Griffith phase, re-entrant spin glass, metamagnetic steps, Hopkinson like peak and also unusual slow relaxation. The M-H curve indicates the presence of competing AFM/FM interactions. The disorder in Tb2CoMnO6 leads to spin frustration at low temperature giving rise to the re-entrant spin glass. Moreover, the field-dependent ac susceptibility studies unraveled the presence of Hopkinson like peak associated with the domain wall motion and the large anisotropy field. The further study yielded that the relaxation associated with this peak is unusually slow.
Magnetic structures and the relationship between spin and charge-orbital orderings of an A-site ordered double-perovskite manganite SmBaMn2O6, an anticipated multiferroic material, were investigated by means of neutron diffraction. The spin arrangement in MnO2 planes perpendicular to the c axis is revealed to be the same as that in the A-site disordered half-doped manganites CE-type but the stacking pattern is found to be different displaying a unique twofold period. The temperature dependence of the superlattice magnetic and nuclear reflections clarifies that the antiferromagnetic spin ordering occurs at a temperature slightly lower than the temperature at which a rearrangement of the charge-orbital orderings occurs. The result evidences that the rearrangement leads the spin ordering. The intensities of the magnetic reflections are found to change across Tf = 10 K, suggesting a spin-flop by 90 [deg.] while keeping the Mn spin ordering pattern unchanged.
We report the observation of spin glass state in the double perovskite oxide Sr$_{2}$FeCoO$_{6}$ prepared through sol-gel technique. Initial structural studies using x rays reveal that the compound crystallizes in tetragonal $I 4/m$ structure with lattice parameters, $a$ = 5.4609(2) AA and $c$ = 7.7113(7) AA. The temperature dependent powder x ray studies reveal no structural phase transition in the temperature range 10 -- 300 K. However, the unit cell volume shows an anomaly coinciding with the magnetic transition temperature thereby suggesting a close connection between lattice and magnetism. Neutron diffraction studies and subsequent bond valence sums analysis show that in Sr$_{2}$FeCoO$_{6}$, the $B$ site is randomly occupied by Fe and Co in the mixed valence states of Fe$^{3+}$/Fe$^{4+}$ and Co$^{3+}$/Co$^{4+}$. The random occupancy and mixed valence sets the stage for inhomogeneous magnetic exchange interactions and in turn, for the spin glass like state in this double perovskite which is observed as an irreversibility in temperature dependent dc magnetization at $T_fsim$ 75 K. Thermal hysteresis observed in the magnetization profile of Sr$_{2}$FeCoO$_{6}$ is indicative of the mixed magnetic phases present. The dynamic magnetic susceptibility displays characteristic frequency dependence and confirms the spin glass nature of this material. Dynamical scaling analysis of $chi(T)$ yields a critical temperature $T_{ct}$ = 75.14(8) K and an exponent $z u$ = 6.2(2) typical for spin glasses. The signature of presence of mixed magnetic interactions is obtained from the thermal hysteresis in magnetization of Sr$_{2}$FeCoO$_{6}$. Combining the neutron and magnetization results of Sr$_2$FeCoO$_6$, we deduce the spin states of Fe to be in low spin while that of Co to be in low spin and intermediate spin.
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.
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