The Griffiths phase-like features and the spin-phonon coupling effects observed in Tb$_2$NiMnO$_6$ are reported. The double perovskite compound crystallizes in monoclinic $P2_1/n$ space group and exhibits a magnetic phase transition at $T_c \sim$ 111 K as an abrupt change in magnetization. A negative deviation from ideal Curie-Weiss law exhibited by 1/$χ(T)$ curves and less-than-unity susceptibility exponents from the power-law analysis of inverse susceptibility are reminiscent of Griffiths phase-like features. Arrott plots derived from magnetization isotherms support the inhomogeneous nature of magnetism in this material. The observed effects originate from antiferromagnetic interactions which arise from inherent disorder in the system. Raman scattering experiments display no magnetic-order-induced phonon renormalization below $T_c$ in Tb$_2$NiMnO$_6$ which is different from the results observed in other double perovskites and is correlated to the smaller size of the rare earth. The temperature evolution of full-width-at-half-maximum for the {\it stretching} mode at 645 cm$^{-1}$ presents an anomaly which coincides with the magnetic transition temperature and signals a close connection between magnetism and lattice in this material.
We put forward double perovskites of the R$_2$NiMnO$_6$ family (with $R$ a rare-earth atom) as a new class of multiferroics on the basis of {\it ab initio} density functional calculations. We show that changing $R$ from La to Y drives the ground-state from ferromagnetic to antiferromagnetic with $\uparrow\uparrow\downarrow\downarrow$ spin patterns. This E$^*$-type ordering breaks inversion symmetry and generates a ferroelectric polarization of few $μC/cm^2$. By analyzing a model Hamiltonian we understand the microscopic origin of this transition and show that an external electric field can be …
We present a comprehensive experimental study of magnetization and magnetocaloric effect (MCE) in double perovskite (DP) materials $R_2$NiMnO$_6$ with $R =$ Pr, Nd, Sm, Gd, Tb, and Dy. While a paramagnetic to ferromagnetic transition, with T$_{\rm C}$ in the range $\sim 100 - 200~$K, is a common feature that can be attributed to the ordering of Mn$^{4+}$ and Ni$^{2+}$ magnetic moments, qualitatively distinct behavior depending on the choice of $R$ is observed at low temperatures. These low-temperature anomalies in magnetization are also manifest in the change in magnetic entropy, $-ΔS_{M}$, wh…
In the family of double perovskites, colossal magnetoresistance (CMR) has been so far observed only in half-metallic ferrimagnets such as the known case Sr$_2$FeMoO$_6$ where it has been assigned to the tunneling MR at grain boundaries due to the half-metallic nature. Here we report a new material-Tl$_2$NiMnO$_6$, a relatively ordered double perovskite stablized by the high pressure and high temperature synthesis-showing CMR in the vicinity of its Curie temperature. We explain the origin of such effect with neutron diffraction experiment and electronic structure calculations that reveal the ma…
Double perovskite (DP) oxide material receive extensive research interest due to exciting physical properties with potential technological application. 3$d$ based DP oxides are promising for exciting physics like magnetodielectric, ferroelectric, Griffith phase etc., specially Co/Mn DPs are gaining much research interest. In this paper we present the study of magnetic phase and transport properties in nano-crystalline Pr$_2$CoMnO$_6$ a 3$d$ based double perovskite compound. This material shows a paramagnetic (PM) to ferromagnetic (FM) phase transition below 173 K marked by a rapid increase in …
First-principles electronic structure calculations have been performed for the double perovskite Bi$_2$CoMnO$_6$ in its non-centrosymmetric polar state using generalized gradient approximation plus Hubbard U approach. We find that while Co is in a high spin state, Mn is in an intermediate spin state. The calculated dynamical charge tensors are anisotropic reflecting a low-symmetry structure of the compound. Magnetic structure dependent phonon frequencies indicate the presence of spin-phonon coupling. Using Berry phase method, we obtain a spontaneous electronic polarization of 5.88 $μC/cm^2$ wh…
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…
Disorder-Induced Griffiths like Phase and Charge Localization in Sr2FeRuO6
South China University of Technology（华南理工大学）；Institute of Engineering and Management, Sector-V（维 sector 工程管理学院）；University of Engineering and Management, Newtown（纽敦工程与管理大学）；Saha Institute of Nuclear Physics, A CI of Homi Bhabha National Institute（萨哈核物理研究所，霍米·巴巴国立学院成员机构）；Department of Physics, Aditya University（阿迪蒂亚大学物理系）
The magnetically ordered states of the A-site ordered perovskite manganites LaBaMn2O6 and YBaMn2O6 have been investigated by muon spin relaxation in zero external magnetic field. Our data reveal striking differences in the nature of the magnetically ordered state of these materials. For LaBaMn2O6, the muSR time-spectra in the ferromagnetic state below ~ 330 K reveal a strongly inhomogeneous phase, reminiscent of a Griffiths phase. Within this magnetically inhomogeneous phase, an antiferromagnetic state develops below 150 K, which displays well defined static internal magnetic fields, but reach…
Transition metal oxides, in particular, 3d or 4d perovskites have provided diverse emergent physics that originates from the coupling of various degrees of freedom such as spin, lattice, charge, orbital, and also disorder. 5d perovskites form a distinct class because they have strong spin-orbit coupling that introduces to the system an additional energy scale that is comparable to bandwidth and Coulomb correlation. Consequent new physics includes novel Jeff = 1/2 Mott insulators, metal-insulator transitions, spin liquids, and topological insulators. After highlighting some of the phenomena app…
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 g…
Electronic structure, electrical transport, dc and ac magnetization properties of the hole substituted (Sr2+) partially B-site disordered double perovskite Pr2-xSrxCoMnO6 system have been investigated. Electronic structure was probed by employing X-ray photoemission spectroscopy (XPS) measurements. The study suggested the presence of mixed valence states of the B-site ions (Co2+/Co3+ and Mn3+/Mn4+) with significant enhancement of the average oxidation states due to hole doping. The mere absence of electronic states near the Fermi level in the valence band (VB) spectra for both of the pure (x=0…
We investigate the unusual phase transitions in SrRuO$_{3}$ and Sr$_{0.5}$Ca$_{0.5}$Ru$_{1-x}$Cr$_{x}$O$_{3}$ (x=0,0.05 and 0.1) employing x-ray diffraction, resistivity, magnetic studies and x-ray photoemission spectroscopy. Our results show the compounds undergo crossover from $itinerant$ ferromagnetism to $localised$ ferromagnetism. The combined studies suggests Ru and Cr to be in 4+ valence state. A Griffith phase and an enhancement in Curie temperature (Tc) from 38 K to 107 K is observed with Cr doping. A shift in the chemical potential towards the valence band is observed with Cr doping.…
