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Register a new userCoexistence of long-ranged charge and orbital order and spin-glass state in single-layered manganites with weak quenched disorder
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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.
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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.
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.
The ac-susceptibility of the electron doped single-layered manganite La$_{1.1}$Sr$_{0.9}$MnO$_4$ is analyzed in detail. A quasi two-dimensional (2$D$) antiferromagnetic (AFM) order with Ising anisotropy is stabilized below $T_N$ $sim$ 80K. We show that below $T_N$, a rare 2$D$ spin-glass (SG) correlation develops with the same Ising anisotropy as the AFM state. Using simple scaling arguments of the droplet model, we derive a scaling form for the ac-susceptibility data of a 2$D$ SG, which our experimental data follows fairly well. Due to simplifications in this 2$D$ case, the proposed scaling form only contains two unknown variables $psi u$ and $tau_0$. Hence, the logarithmic growth law of the SG correlation predicted by the droplet model is convincingly evidenced by the scaling of our experimental data. The origin and nature of this 2$D$ SG state is also discussed.
As a sister compound and isostructural of MnBi2Te4, the high quality MnSb2Te4 single crystals are grown via solid-state reaction where prolonged annealing and narrow temperature window play critical roles on account of its thermal metastability. X-ray diffraction analysis on MnSb2Te4 single crystals reveals pronounced cation intermixing, 28.9(7)% Sb antisite defects on the Mn (3a) site and 19.3(6)% Mn antisite defects on the Sb (6c) site, compared with MnBi2Te4. Unlike antiferromagnetic (AFM) nature MnBi2Te4, MnSb2Te4 contains magnetic and antiferromagnetic competition and exhibits a spin glass (SG) state below 24 K. Its magnetic hysteresis, anisotropy, and relaxation process are investigated in detail with DC and AC magnetization measurements. Moreover, anomalous Hall effect as a p-type conductor is demonstrated through transport measurements. This work grants MnSb2Te4 a possible access to the future exploration of exotic quantum physics by removing the odd/even layer number restraint in intrinsic AFM MnBi2Te4-family materials as a result of the crossover between its magnetism and potential topology in the Sb-Te layer.
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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