An effort is made to study the contrast in magnetic behavior resulting from minimal disorder introduced by substitution of 2.5% Ga or Al in Mn-site of La${_{0.9}}$Sr$_{0.1}$MnO${_3}$. It is considered that Ga or Al selectively creates disorder within the orbital domains or on its walls, causing enhancement of Griffiths phase (GP) singularity for the former and disappearance of it in the later case. It is shown that Ga replaces Mn$^{3+}$ which is considered to be concentrated within the domains, whereas Al replaces Mn$^{4+}$ which is segregated on the hole-rich walls, without causing any significant effect on structure or ferromagnetic transition temperatures. Thus, it is presumed that the effect of disorder created by Ga extend across the bulk of the domain having correlation over similar length-scale resulting in enhancement of GP phenomenon. On the contrary, effect of disorder created by Al remains restricted to the walls resulting in the modification of the dynamics arising from the domain walls and suppresses the GP. Moreover contrasting features are observed in the low temperature region of the compounds; a re-entrant spin glass like behavior is observed in the Ga doped sample, while the observed characteristics for the Al doped sample is ascribed only to modified domain wall dynamics with the absence of any glassy phase. Distinctive features in third order susceptibility measurements reveals that the magnetic ground state of the entire series comprises of orbital domain states. These observations bring out the role of the nature of disorder on GP phenomenon and also reconfirms the character of self-organization in low-doped manganites.
We show that specific heat C$_p$ has non-Debye behavior for glassy states in half-doped manganites. Irrespective of the magnetic order or electronic states, these magnetic glasses have higher C$_p$ compared to their equilibrium counterparts. The excess C$_p$ contributed by the glassy state varies linearly with temperature similar to conventional glasses indicating tunneling in the two-level systems. These glassy states show signature of zero point entropy. Magnetic glasses can be produced simply by different field cooling protocols and may be considered ideal magnetic counterpart of the conven…
This paper reports the observations of long-time relaxation, aging, and temperature memory behaviors of resistance and magnetization in the ferromagnetic state of a polycrystalline La0.7Ca0.3Mn0.925Ti0.075O3 compound. The observed glassy dynamics of the electrical transport appears to be magnetically originated and has a very close association with the magnetic glassiness of the sample. Phase separation and strong correlation between magnetic interactions and electronic conduction play the essential roles in producing such a resistive glassiness. We explain the observed effects in terms of a c…
We report the existence of Griffiths phase (GP) over a wide range of $x$ in La$_{0.6}$Sr$_{0.4}$Mn$_{1-x}$Co$_x$O$_3$, the solid solution of ferromagnetic (FM) La$_{0.6}$Sr$_{0.4}$MnO$_3$ and La$_{0.6}$Sr$_{0.4}$CoO$_3$, from magnetization measurements. In this compound, GP arises due to the quenching of randomly distributed Co-O-Mn antiferromagnetic bonds in the FM background. In contrary to divalent doped manganites, GP in the present system can exist entirely in the metallic state above $T_C$ (for $x$$<$0.10). Based on the present study, a magnetoelectronic phase diagram is drawn.
We report here the magnetic properties of electron-doped Sm1-xCaxMnO3 manganites with the doping level of x=0.91. Exchange bias effect has been observed in Sm0.09Ca0.91MnO3 nanomanagnites system and can be tuned by the strength of cooling magnetic field (Hcool). The values of exchange bias parameter i.e. exchange bias fields (HE), coercivity (HC), remanence asymmetry (ME) and magnetic coercivity (MC) are found to strongly depend on Hcool. The larger effective magnetic moments and deviation of inverse susceptibility (\c{hi}-1) from Curie-Weiss law indicate the possible existence of Griffiths ph…
The finite-size effect on the evolution of Griffiths phase (GP) is studied using nanoparticles of half-doped manganite Pr$_{0.5}$Sr$_{0.5}$MnO$_{3}$ with different average particle sizes but having similar structural parameters. All the samples exhibit pronounced GP behavior. With reducing particle size, the Griffiths temperature remains almost unchanged but the characteristic critical temperature $T_c^R$ decreases and the GP properties are strengthened. It is noteworthy that the shift of $T_c^R$ follows finite-size scaling with the particle size revealing an exotic interplay between the GP pr…
The single layered manganite Pr$_{0.22}$Sr$_{1.78}$MnO$_4$ undergoes structural transition from high temperature tetragonal phase to low temperature orthorhombic phase below room temperature. The orthorhombic phase was reported to have two structural variants with slightly different lattice parameters and Mn-3$d$ levels show orbital ordering within both the variants, albeit having mutually perpendicular ordering axis. In addition to orbital ordering, the orthorhombic variants also order antiferromagnetically with different Néel temperatures. Our magnetic investigation on the polycrystalline sa…
The large, so-called colossal, magnetoresistivity of doped manganese oxides based on LaMnO3 has attracted considerable attention, but only one unusual feature of the ferromagnetic transition in these compounds. We examine in this paper the progression of magnetic and thermodynamic behavior as the transition temperature is made to vary from 360 K to 218 K by changing the divalent dopant. Single crystals of La_{0.7}Sr_{0.3}MnO3, as is well known, show modest magnetoresistivity and conventional critical behavior. La$_{0.7}$Pb$_{0.3}$ Mn$O_3$, and to an even greater extent, La$_{0.7}$Ca$_{0.3}$MnO…
The glassy response of thin films of La0.8Ca0.2MnO3 to external magnetic and gated electrostatic fields in a field-effect geometry has been studied at low temperatures. A hierarchical response with irreversible memory effects, non-ergodic time evolution, aging and annealing behavior of the resistance suggest that the dynamics are governed by strain relaxation for both electronic and magnetic perturbations. Cross-coupling of charge, spin, and strain have been exploited to tune the coercivity of an ultrathin manganite film by electrostatic gating.
Antiferromagnetic-insulating(AF-I) and the ferromagnetic-metallic(FM-M) phases coexist in various half-doped manganites over a range of temperature and magnetic field, and this is often believed to be an essential ingredient to their colossal magnetoresistence. We present magnetization and resistivity measurements on Pr(0.5)Ca(0.5)Mn(0.975)Al(0.025)O(3) and Pr(0.5)Sr(0.5)MnO(3) showing that the fraction of the two coexisting phases at low-temperature in any specified measuring field H, can be continuously controlled by following designed protocols traversing field-temperature space; for both m…
It is now widely accepted that the magnetic transition in doped manganites that show large magnetoresistance is a type of percolation effect. This paper demonstrates that the transition should be viewed in the context of the Griffiths phase that arises when disorder suppresses a magnetic transition. This approach explains unusual aspects of susceptibility and heat capacity data from a single crystal of La$_{0.7}$Ca$_{0.3}$MnO$_{3}.$
We report a comprehensive investigation of La0.2Pr0.4Ca0.4MnO3 to clarify the micrometre scale phase separation phenomenon in the mixed valent manganite (La,Pr,Ca)MnO3. The compound shows multiple magnetic transitions, in which the charge-ordered state is converted into a ferromagnetic state in steps with the application of a magnetic field. The ac susceptibility measurements show that the glassy transition at low temperatures does not depend on the frequency, thus indicating the absence of any spin glass behaviour. Magnetization as well as heat capacity measurements indicate that this low tem…
The discovery of novel structural and physical properties in the $A$-site ordered manganite $R$BaMn$_{2}$O$_{6}$ ($R$ = Y and rare earth elements) has demanded new comprehension about perovskite manganese oxides. In the present study, the $A$-site disordered form, $R_{0.5}$Ba$_{0.5}$MnO$_{3}$, has been investigated and compared with both $R$BaMn$_{2}$O$_{6}$ and $R_{0.5}A_{0.5}$MnO$_{3}$ ($A$: Sr, Ca) in the structures and electromagnetic properties. $R_{0.5}$Ba$_{0.5}$MnO$_{3}$ has a primitive cubic perovskite cell in the structure and magnetic glassy states are dominant as its ground state, …
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…
Impurity effects on the stability of a ferromagnetic metallic state in a bicritical-state manganite, (La0.7Pr0.3)0.65Ca0.35MnO3, on the verge of metal-insulator transition have been investigated by substituting a variety of transition-metal atoms for Mn ones. Among them, Fe doping exhibits the exceptional ability to dramatically decrease the ferromagnetic transition temperature. Systematic studies on the magnetotransport properties and x-ray diffraction for the Fe-doped crystals have revealed that charge-orbital ordering evolves down to low temperatures, which strongly suppresses the ferromagn…
The exchange bias (EB) in LaMn_{0.7}Fe_{0.3}O_3 is observed by the negative shift and training effect of the hysteresis loops, while the sample was cooled in external magnetic field. The analysis of cooling field dependence of EB gives the size of the ferromagnetic (FM) cluster ~ 25 Angstrom, where the magnetic anisotropy of FM cluster is found two order of magnitude higher than the FM bulk manganites. We propose that the nanoscale FM clusters are embedded in the glassy magnetic host with EB at the FM/glassy magnetic interface.
The physics underlying the complex glassy phenomena, which accompany the formation of polarons in optimally doped manganites (ODM) is a cumbersome issue with many unexplained aspects. In this article we present $^{139}$La and $^{55}$Mn NMR in the temperature range 80K - 900K of ODM La$_{0.67}$Ca$_{0.33}$MnO$_3$. We show that local lattice distortions, established in the Paramagnetic (PM) phase for $T<700$K, induce a genuine spin-glass state, which for $T<T_c$ consolidates with the Ferromagnetic (FM) state into a single thermodynamic phase. Comparative NMR experiments on La$_{0.77}$Ca$_{0.23}$M…
The analysis of phonon anomalies provides valuable information about the cooperative dynamics of lattice, spin and charge degrees of freedom. Significant is the anomalous temperature dependence of the external modes observed in La$_{2/3}$Sr$_{1/3}$MnO$_{3}$ (LSMO) films. The two external modes merge close to the ferromagnetic to paramagnetic transition at $T_C$ and, moreover, two new modes evolve in this temperature range with strong resonances at slightly higher frequencies. We propose that this observed phonon metamorphosis probes the inhomogeneous Jahn-Teller distortion, manifest on the tem…
We have investigated magnetic, electrical and thermal transport properties (Seebeck effect and thermal conductivity) of LaSr$_{2}$Mn$_{2-y}$Cr$_{y}$O$_{7}$ polycrystalline samples ($y$=0.1, 0.2, 0.4 and 0.6). The Cr$^{3+}$ substitution for Mn$^{3+}$ sites causes a removal of $d_{x^2-y^2}$ orbital of $e_g$-electron resulting in a volume shrinkage of lattice. Magnetic measurements reveal the appearance of a glassy behavior for Cr-doped samples, accompanied by both a collapse of the A-type antiferromagnetic structure and the growth of ferromagnetic clusters. Cr-doping effect on electrical transpo…
An attempt is made to resolve the controversy related to the low temperature phase (ground state) of the low-doped ferromagnetic (FM)- insulator(I) manganite through bulk magnetic measurements on La${_{0.9}}$Sr$_{0.1}$MnO${_3}$ sample. It is shown that the FM phase, formed out of well defined transition in the low-doped system, becomes inhomogeneous with decrease in temperature. This inhomogeniety is considered to be an outcome of the formation of orbital domain state of e$_g$-electrons having hole rich (metallic) walls separating the hole deficient (insulating) regions. The resulting complexi…
We show that Pr${_{0.5}}$Ca$_{0.5}$MnO${_3}$ with 2.5% Al substitution and La${_{0.5}}$Ca$_{0.5}$MnO${_3}$ (LCMO) exhibit qualitatively similar and visibly anomalous M-H curves at low temperature. Magnetic field causes a broad first-order but irreversible antiferromagnetic (AF)-insulating (I) to ferromagnetic (FM)-metallic (M) transition in both and gives rise to soft FM state. However, the low temperature equilibrium state of Pr$_{0.5}$Ca$_{0.5}$Mn$_{0.975}$Al$_{0.025}$O$_3$ (PCMAO) is FM-M whereas that of LCMO is AF-I. In both the systems the respective equilibrium phase coexists with the ot…
The metal-insulator transition, and the associated magnetic transition, in the colossal magnetoresistance (CMR) regime of the one-orbital model for manganites is here studied using Monte Carlo (MC) techniques. Both cooperative oxygen lattice distortions and a finite superexchange coupling among the $t_{\rm 2g}$ spins are included in our investigations. Charge and spin correlations are studied. In the CMR regime, a strong competition between the ferromagnetic metallic and antiferromagnetic charge-ordered insulating states is observed. This competition is shown to be important to understand the …
We investigate the dynamics of magnetization in the phase separated (PS) state after introducing the quenched disorder at the Mn-site of a manganite around half doping. The compound, Pr$_{0.5}$Sr$_{0.5}$Mn$_{0.925}$Ga$_{0.075}$O$_{3}$, exhibits PS with the coexistence of ferromagnetic (FM) and antiferromagnetic (AFM) clusters where the size of the FM clusters is substantially reduced due to the disorder introduced by nonmagnetic Ga substitution. At low temperature, the system develops a new magnetic anomaly, which is marked by a peak in the zero field cooled magnetization. Detailed study of li…
Cobalt based sulphides of compositional formula Co$ _{3} $A$ _{2} $S$ _{2} $ (A = Sn and In) are endowed with frustrated kagome lattice structure and a plethora of novel phenomena determined from the topological band structure. Here-in, we report on the detailed exploration of anisotropic magnetic properties of single crystals of ferromagnetic compound Co$ _{3} $Sn$ _{2} $S$ _{2} $ under magnetic field $H$ applied along the c-axis $(H\parallel c)$ and the ab-plane $(H\parallel ab)$. A low temperature clustered-glassy magnetic behaviour is revealed in field-cooled and zero field-cooled magnetiz…
Phenomenological models for the antiferromagnetic (AF) vs. d-wave superconductivity competition in cuprates are studied using conventional Monte Carlo techniques. The analysis suggests that cuprates may show a variety of different behaviors in the very underdoped regime: local coexistence or first-order transitions among the competing orders, stripes, or glassy states with nanoscale superconducting (SC) puddles. The transition from AF to SC does not seem universal. In particular, the glassy state leads to the possibility of "colossal'' effects in some cuprates, analog of those in manganites. U…
The influence of quenched disorder on the competition between ordered states separated by a first-order transition is investigated. A phase diagram with features resembling quantum-critical behavior is observed, even using classical models. The low-temperature paramagnetic regime consists of coexisting ordered clusters, with randomly oriented order parameters. Extended to manganites, this state is argued to have a colossal magnetoresistance effect. A scale T* for cluster formation is discussed. This is the analog of the Griffiths temperature, but for the case of two competing orders, producing…
We report results of magnetization and ac susceptibility measurements down to very low fields on a single crystal of the perovskite manganite, La$_{0.82}$Ca$_{0.18}$MnO$_3$. This composition falls in the intriguing ferromagnetic insulator region of the manganite phase diagram. In contrast to earlier beliefs, our investigations reveal that the system is magnetically (and in every other sense) single-phase with a ferromagnetic ordering temperature of $\sim$ 170 K. However, this ferromagnetic state is magnetically frustrated, and the system exhibits pronounced glassy dynamics below 90 K. Based on…
We study the effects of short-range correlated disorder arising from chemical dopants or local lattice distortions, on the ferromagnetism of 3d double exchange systems. For this, we integrate out the carriers and treat the resulting disordered spin Hamiltonian within local random phase approximation, whose reliability is shown by direct comparison with Monte Carlo simulations. We find large scale inhomogeneities in the charge, couplings and spin densities. Compared with the homogeneous case, we obtain larger Curie temperatures ($T_{C}$) and very small spin stiffnesses ($D$). As a result, large…
