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In this paper, we mainly focus on the magnetic and magnetocaloric features of La2-xDyxNiMnO6 double perovskites. Their magnetocaloric properties are investigated in terms of both entropy and adiabatic temperature changes. In contrast to early works, it was found that the Dy2NiMnO6 compound unveils dominant antiferromagnetic interactions under very low magnetic fields. The ordering of its Dy3+ magnetic moments is associated with a giant magnetocaloric effect at very low temperatures, while the established ferromagnetic Ni-O-Mn super-exchange interactions close to 100 K give rise to a moderate magnetocaloric level, only. On the other hand, the doping of Dy2NiMnO6 with high amounts of large-size rare earth elements such as La would enable us to cover an unusually wide magnetocaloric temperature range going from the liquid helium temperature up to room-temperature. More interestingly, the presence of both ordered and disordered ferromagnetic phases in La1.5Dy0.5NiMnO6 maintains constant the isothermal entropy changes over a temperature span of about 200 K, being a favorable situation from a practical point of view., Comment: Accepted for publication in Journal of Physics: D, 2019

X-ray absorption spectroscopy (XAS) is one of the most widely used experimental techniques to study the electronic and spatial structure of materials. Fluorescence yield mode is bulk-sensitive, but has several serious problems coming from saturation effects. In this study, we show the usefulness of partial fluorescence yields in addressing these problems. We discuss the different behaviors of La2NiMnO6 and LiMnO2 at the Mn 2p absorption edges. The total fluorescence yield produces misleading spectra for LiMnO2 due to the absence of high-Z (Z: atomic number) elements. We conclude that the measurement of the inverse partial fluorescence yield is essential in studies of LiMnO2, which is a hotly debated Li-ion battery material., Comment: 3 pages, 3 figures

Ultrasonic velocity measurements on the magnetoelectric multiferroic compound CuFeO2 reveal that the antiferromagnetic transition observed at TN1 = 14 K might be induced by an R-3m -> C2/m pseudoproper ferroelastic transition (G. Quirion, M. J. Tagore, M. L. Plumer, O. A. Petrenko, Phys. Rev. B 77, 094111 (2008)). In that case, the group theory states that the order parameter associated with the structural transition must belong to a two dimensional irreducible representation Eg (x^2 - y^2, xy). Since this type of transition can be driven by a Raman Eg mode, we performed Raman scattering measurements on CuFeO2 between 5 K and 290 K. Considering that the isostructural multiferroic compound CuCrO2 might show similar structural deformations at the antiferromagnetic transition TN1 = 24.3 K, Raman measurements have also been performed for comparison. At ambient temperature, the Raman modes in CuFeO2 are observed at omega_Eg = 352 cm^-1 and omega_Ag = 692 cm^-1, while these modes are detected at omega_E_g = 457 cm^-1 and omega_Ag = 709 cm^-1 in CuCrO2. The analysis of the temperature dependence of modes shows that the frequency of all modes increases down to 5 K. This typical behavior can be attributed to anharmonic phonon-phonon interactions. These results clearly indicate that none of the Raman active modes observed in CuFeO2 and CuCrO2 drive the pseudoproper ferroelastic transition observed at the N\'eel temperature TN1. Finally, a broad band at about 550 cm^-1 observed in the magnetoelectric phase of CuCrO2 below TN2 could be attributed to a magnon mode., Comment: 11 pages, 5 figures

The temperature dependence of phonon excitations and the presence of spin phonon coupling in polycrystalline Pr2NiMnO6 samples were studied using micro-Raman spectroscopy and magnetometry. Magnetic properties show a single ferromagnetic-to-paramagnetic transition at 228 K and a saturation magnetization close to 4.95 \muB/f.u.. Three distinct Raman modes at 657, 642, and 511 cm-1 are observed. The phonon excitations show a clear hardening due to anharmonicity from 300 K down to 10 K. Further, temperature dependence of the 657 cm-1 mode shows only a small softening. This reflects the presence of a relatively weak spin-phonon coupling in Pr2NiMnO6 contrary to other double perovskites previously studied., Comment: 10 pages, 4 figs

In the quest for novel magnetoelectric materials, we have grown, stabilized and explored the properties of La3BAlMnO9 (B = Co or Mn) thin films. In this paper, we report the influence of the growth parameters that promote B/Al/Mn ordering in the pseudo-cubic unit cell and their likely influence on the magnetic and multiferroic properties. The temperature dependence of the magnetization shows that La3CoAlMnO9 is ferromagnetic up to 190 K while La3NiAlMnO9 shows a TC of 130 K. The behavior of these films are compared and contrasted with related La2BMnO6 double perovskites. It is observed that the insertion of AlO6 octahedra between CoO6 and MnO6 suppresses significantly the strength of the superexchange interaction, spin-phonon and spin-polar coupling., Comment: 13 pages, 3 figs

Despite the great technological and scientific importance, a well-controlled coupled behavior in magnetoelectric multiferroic materials at room temperature remains challenging. We demonstrate that the self-ordered A2BBO6 (e.g., A = La, B = Mn, and B = Ni) double perovskites provide a unique alternative opportunity to control and/or to induce such behavior in oxides. In this paper, we outline and discuss the various challenges and bottleneck issues related to this class of materials using La2NiMnO6 as a prototype. Details of the synthesis strategies, using pulsed laser deposition as a central tool, to obtain a meticulous control over cation ordering is illustrated. The possible impact of Ni/Mn cation ordering on the magnetic ground states, ferromagnetic transition temperature, phonon behavior, and spin-phonon coupling are presented. Our results are also compared with the current literature on related compounds., Comment: 12 pages, 3 figures

We report the influence of Ni/Mn ordering on the spin-phonon coupling in multifunctional La2NiMnO6. Three types of films with different levels of structural order, including long-range Ni/Mn cation order, cation disorder, and an admixture of the ordered and disordered phases, are compared by polarized micro-Raman spectroscopy and magnetometry. Each film displays a strong dependence on the polarization configuration and a unique set of Raman active phonon excitations. Long-range cation ordering results in the splitting of Raman active phonon peaks because of Brillouin zone folding and lowering symmetry. Phonon mode softening begins clearly at a distinct temperature for each sample revealing a strong spin-lattice interaction. It follows closely the magnetization curve in ordered films. Unlike the admixture and the ordered films, softening behavior is strongly suppressed in the cation-disordered films. These differences may be understood based on the variation in amplitude of the spin-spin correlation functions due to the local Ni/Mn cation ordering., Comment: 17 pages, 7 figs

We report and compare the structural, magnetic, and optical properties of ordered La2NiMnO6 thin films and its disordered LaNi0.5Mn0.5O3 counterpart. An x-ray diffraction study reveals that the B-site Ni/Mn ordering induces additional XRD reflections as the crystal symmetry is transformed from a pseudocubic perovskite unit cell in the disordered phase to a monoclinic form with larger lattice parameters for the ordered phase. Polarized Raman spectroscopy studies reveal that the ordered samples are characterized by additional phonon excitations that are absent in the disordered phase. The appearance of these additional phonon excitations is interpreted as the clearest signature of Brillouin zone folding as a result of the long-range Ni/Mn ordering in La2NiMnO6. Both ordered and disordered materials display a single ferromagnetic-to-paramagnetic transition. The ordered films display also a saturation magnetization close to 4.8 mB/f.u. and a transition temperature (FM-TC) around 270 K, while the disordered ones have only a 3.7 mB/f.u. saturation magnetization and a FM-TC around 138 K. The differences in their magnetic behaviours are understood based on the distinct local electronic configurations of their Ni/Mn cations., Comment: 15 pages, 5 figs

Millimeter size single crystals of double perovskite La2NiMnO6 (LNMO) were grown by the High Temperature Solution Growth Method. The magnetic measurements and polarized Raman spectra between 5 and 350K provide evidence that the crystals have high degree of Ni(2+)/Mn(4+)ordering, small amount of lattice defects and highest Tc = 288K reported so far for ferromagnetic double perovskites. At a microscopic level the crystals are heavily twinned and the effect of twinning on the Raman spectra is analyzed in detail., Comment: 5 pages, 4 figures

Double perovskites provide a unique opportunity to induce and control multiferroic behaviors in oxide systems. The appealing possibility to design materials with a strong coupling between the magnetization and the polarization fields may be achieved in this family since these magnetic insulators can present structural self-ordering in the appropriate growth conditions. We have studied the functional properties of La2CoMnO6 and Bi2CoMnO6 epitaxial thin films grown by pulsed laser deposition. Cation-ordered La2CoMnO6 films display a magnetic Curie temperature of 250 K while cation-disordered Bi2CoMnO6 films present ferromagnetism up to ~ 800 K. Such high transition temperature for magnetic ordering can be further tuned by varying the strain in the films indicating an important contribution from the structural characteristics of the materials. Our approach might be generalized for other oxide systems. At this end, our results are compared with other multiferroic systems. The roles of various cations, their arrangements and structural effects are further discussed., Comment: 12 pages, 5 figs

Ferromagnetic La3NiAlMnO9 (LNAMO) and La3CoAlMnO9 (LCAMO) triple-perovskite thin films are stabilized in the 750-860 oC temperature range in 100 to 900 mTorr O2 pressure range using pulsed-laser deposition. The LCAMO and LNAMO films exhibit ferromagnetism up to 190 K and 130 K respectively. The structural, optical and magnetic properties of these films demonstrate that the B-site 3d-cations, Al, Mn and Co or Ni ions, are structurally short-range ordered. The strong spin-lattice-polarization coupling in LCAMO is evidenced by the temperature dependence of the dielectric constant and the softening of the phonon frequencies starting in the vicinity of the ferromagnetic-to-paramagnetic phase transition mimicking the behaviours of La2CoMnO6 double perovskite., Comment: 11 pages, 4 figs