No Arabic abstract
Fundamental and harmonic magneto-dielectricity studied for varied perovskite systems-- Pb0.98Gd0.02(Mg1/3Nb2/3)0.995O3 (A-site co-doped PGMN magneto-relaxor), La0.95Ca0.05CoO3 (A-site doped spin-state LCCO), and La2NiMnO6 (double-perovskite LNMO multiglass) characterize intricately polarized phases. First-harmonic signal ({epsilon}2) of magnetically co-doped PGMN manifests finite polarization P(H) below 270K, corroborated by the measured remnant P-E traces. Second-harmonic ({epsilon}3) reveals the effect of random E-fields causing electrical vitreousity, latter indicated by the divergent timescale of the fundamental response. LCCO features mixed-dipoles phase over appreciable temperature window, affiliated to the coexistent low-spins (LS) and intermediate-spins (IS). Across the 65K-start of IS-to-LS state transition (SST), dc- and ac-conductivities of LCCO exhibit mechanism-changeovers whereas the harmonic susceptibilities evidence IS/LS-interfacial hyper-polarizations. Below the 30K-end of SST, harmonics corroborate the vitreous phase of dipoles in the LS-matrix state. In the LNMO, positive and negative (dual) magneto-dielectricity observed is respectively attributed to the charge-hopping between Ni2+ and Mn4+ ions and the interfacial polarization. Second-harmonic signal here also features dispersion corresponding to the activation energy required for the electron transfer between Ni- and Mn-cations. Results from three different perovskite systems signify the combined importance of first- and second-harmonics, for a detailed understanding of electrical configurations.
Frequency-dependent and temperature-dependent dielectric measurements are performed on double perovskite Tb$_2$NiMnO$_6$. The real ($epsilon_1$) and imaginary ($epsilon_2$) parts of dielectric permittivity show three plateaus suggesting dielectric relaxation originating from bulk, grain boundaries and the sample-electrode interfaces respectively. The temperature and frequency variation of $epsilon_1$ and $epsilon_2$ are successfully simulated by a $RC$ circuit model. The complex plane of impedance, $Z$-$Z$, is simulated using a series network with a resistor $R$ and a constant phase element. Through the analysis of frequency-dependent dielectric constant using modified-Debye model, different relaxation regimes are identified. Temperature dependence of dc conductivity also presents a clear change in slope at, $T^*$. Interestingly, $T^*$ compares with the temperature at which an anomaly occurs in the phonon modes and the Griffiths temperature for this compound. The components $R$ and $C$ corresponding to the bulk and the parameter $alpha$ from modified-Debye fit tend support to this hypothesis. Though these results cannot be interpreted as magnetoelectric coupling, the relationship between lattice and magnetism is marked.
We have investigated spin and orbital magnetic moments of the Re 5d ion in the double perovskites A2FeReO6 (A = Ba, Sr, Ca) by X-ray magnetic circular dichroism (XMCD) at the Re L(2,3) edges. In these ferrimagnetic compounds an unusually large negative spin and positive orbital magnetic moment at the Re atoms was detected. The presence of a finite spin magnetic moment in a non-magnetic double perovskite as observed in the double perovskite Sr2ScReO6 proves that Re has also a small, but finite intrinsic magnetic moment. We further show for the examples of Ba and Ca that the usually neglected alkaline earth ions undoubtedly also contribute to the magnetism in the ferrimagnetic double perovskites.
Dielectric study on Ca3Mn2O7 features relaxor-like segmented dynamics below the antiferromagnetic ordering. Dipolar relaxations of different origin are spectrally resolved exhibiting distinct H-field alterations. This identifies their allegiance to different magnetic sub-phases and establishes dual coupling of electrical, magnetic, and structural degrees of freedom. Further, strong spin-lattice coupling has been affirmed with Raman spectroscopy across the magnetic ordering. Short-range electrical correlations collaterally cause measurable harmonic dielectric response in the system. The c{hi}_3^e-susceptibility signal yields genuine harmonic magneto-dielectricity, consistent with but exhibiting two orders of magnitude larger H-field effect, vis-`a-vis that obtained in the fundamental dielectric constant {epsilon}.
Recently, the iridate double perovskite Sr$_2$YIrO$_6$ has attracted considerable attention due to the report of unexpected magnetism in this Ir$^{5+}$ (5d$^4$) material, in which according to the J$_{eff}$ model, a non-magnetic ground state is expected. However, in recent works on polycrystalline samples of the series Ba$_{2-x}$Sr$_x$YIrO$_6$ no indication of magnetic transitions have been found. We present a structural, magnetic and thermodynamic characterization of Sr$_2$YIrO$_6$ single crystals, with emphasis on the temperature and magnetic field dependence of the specific heat. Here, we demonstrate the clue role of single crystal X-ray diffraction on the structural characterization of the Sr$_2$YIrO$_6$ double perovskite crystals by reporting the detection of a $sqrt{2}a times sqrt{2}a times 1c$ supercell, where $a$, $b$ and $c$ are the unit cell dimensions of the reported monoclinic subcell. In agreement with the expected non-magnetic ground state of Ir$^{5+}$ (5d$^4$) in Sr$_2$YIrO$_6$, no magnetic transition is observed down to 430~mK. Moreover, our results suggest that the low temperature anomaly observed in the specific heat is not related to the onset of long-range magnetic order. Instead, it is identified as a Schottky anomaly caused by paramagnetic impurities present in the sample, of the order of $n sim 0.5(2)$ %. These impurities lead to non-negligible spin correlations, which nonetheless, are not associated with long-range magnetic ordering.
Doping is a widely used method to tune physical properties of ferroelectric perovskites. Since doping can induce charges due to the substitution of certain elements, charge effects shall be considered in doped samples. To understand how charges can affect the system, we incorporate the dipole-charge interaction into our simulations, where the pinched hysteresis loops can well be reproduced. Two charge compensation models are proposed and numerically investigated to understand how lanthanum doping affect BaTiO$_{3}$s ferroelectric phase transition temperature and hysteresis loop. The consequences of the two charge compensation models are compared and discussed.