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Register a new userColossal magnetoresistance without phase separation: Disorder-induced spin glass state and nanometer scale orbital-charge correlation in half doped manganites
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The magnetic and electrical properties of high quality single crystals of $A$-site disordered (solid solution) Ln$_{0.5}$Ba$_{0.5}$MnO$_3$ are investigated near the phase boundary between the spin glass insulator and colossal-magnetoresistive ferromagnetic metal, locating near Ln = Sm. The temperature dependence of the ac-susceptibility and the x-ray diffuse scattering of Eu$_{0.5}$Ba$_{0.5}$MnO$_3$ are analyzed in detail. The uniformity of the random potential perturbation in Ln$_{0.5}$Ba$_{0.5}$MnO$_3$ crystals with small bandwidth yields, rather than the phase separation, an homogeneous short ranged charge/orbital order which gives rise to a nearly-atomic spin glass state. Remarkably, this microscopically disordered ``CE-glass state alone is able to bring forth the colossal magnetoresistance.
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High resolution topographic images obtained by scanning tunneling microscope in the insulating state of Pr0.68Pb0.32MnO3 single crystals showed regular stripe-like or zigzag patterns on a width scale of 0.4 - 0.5 nm confirming a high temperature polaronic state. Spectroscopic studies revealed inhomogeneous maps of zero-bias conductance with small patches of metallic clusters on length scale of 2 - 3 nm only within a narrow temperature range close to the metal-insulator transition. The results give a direct observation of polarons in the insulating state, phase separation of nanometer-scale metallic clusters in the paramagnetic metallic state, and a homogeneous ferromagnetic state.
Phase diagrams in the plane of $r_A$ (the average ionic radius, related to one-electron bandwidth $W$) and $sigma^2$ (the ionic radius variance, measuring the quenched disorder), or ``bandwidth-disorder phase diagrams, have been established for perovskite manganites, with three-dimensional (3$D$) Mn-O network. Here we establish the intrinsic bandwidth-disorder phase diagram of half-doped layered manganites with the two-dimensional (2$D$) Mn-O network, examining in detail the ``mother state of the colossal magnetoresistance (CMR) phenomenon in crystals without ferromagnetic instability. The consequences of the reduced dimensionality, from 3$D$ to 2$D$, on the order-disorder phenomena in the charge-orbital sectors are also highlighted.
The relationship between orbital and spin degrees of freedom in the single-crystals of the hole-doped Pr$_{1-x}$Ca$_{1+x}$MnO$_4$, 0.3 $leq$ $x$ $leq$ 0.7, has been investigated by means of ac-magnetometry and charge transport. Even though there is no cation ordering on the $A$-site, the quenched disorder is extremely weak in this system due to the very similar ionic size of Pr$^{3+}$ and Ca$^{2+}$. A clear asymmetric response of the system to the under- (respective over-) hole doping was observed. The long-ranged charge-orbital order established for half doping ($x$=0.5) subsists in the over-doping case ($x$ $>$ 0.5), albeit rearranged to accommodate the extra holes introduced in the structure. The charge-orbital order is however destabilized by the presence of extra localized electrons (under-doping, $x$ $<$ 0.5), leading to its disappearance below $x$=0.35. We show that in an intermediate under-doped region, with 0.35 $leq$ $x$ $<$ 0.5, the ``orbital-master spin-slave relationship commonly observed in half-doped manganites does not take place. The long-ranged charge-orbital order is not accompanied by an antiferromagnetic transition at low temperatures, but by a frustrated short-ranged magnetic state bringing forth a spin-glass phase. We discuss in detail the nature and origin of this spin-glass state, which, as in the half-doped manganites with large quenched disorder, is not related to the macroscopic phase separation observed in crystals with minor defects or impurities.
The correlation between colossal magnetocapacitance (CMC) and colossal magnetoresistance (CMR) in CdCr2S4 system has been revealed. The CMC is induced in polycrystalline Cd0.97In0.03Cr2S4 by annealing in cadmium vapor. At the same time, an insulator-metal transition and a concomitant CMR are observed near the Curie temperature. In contrast, after the same annealing treatment, CdCr2S4 displays a typical semiconductor behavior and does not show magnetic field dependent dielectric and electric transport properties. The simultaneous occurrence or absence of CMC and CMR effects implies that the CMC in the annealed Cd0.97In0.03Cr2S4 could be explained qualitatively by a combination of CMR and Maxwell-Wagner effect.
A central line of inquiry in condensed matter science has been to understand how the competition between different states of matter give rise to emergent physical properties. Perhaps some of the most studied systems in this respect are the hole-doped LaMnO$_3$ perovskites, with interest in the past three decades being stimulated on account of their colossal magnetoresistance (CMR). However, phase segregation between ferromagnetic (FM) metallic and antiferromagnetic (AFM) insulating states, which itself is believed to be responsible for the colossal change in resistance under applied magnetic field, has until now prevented a full atomistic level understanding of the orbital ordered (OO) state at the optimally doped level. Here, through the detailed crystallographic analysis of the hole-doped phase diagram of a prototype system, we show that the superposition of two distinct lattice modes gives rise to a striped structure of OO Jahn-Teller active Mn$^{3+}$ and charge disordered (CD) Mn$^{3.5+}$ layers in a 1:3 ratio. This superposition leads to an exact cancellation of the Jahn-Teller-like oxygen atom displacements in the CD layers only at the 3/8th doping level, coincident with the maximum CMR response of the manganties. Furthermore, the periodic striping of layers containing Mn$^{3.5+}$, separated by layers of fully ordered Mn$^{3+}$, provides a natural mechanism though which long range OO can melt, a prerequisite for the emergence of the FM conducting state. The competition between insulating and conducting states is seen to be a key feature in understanding the properties in highly correlated electron systems, many of which, such as the CMR and high temperature superconductivity, only emerge at or near specific doping values.
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