Bridging charge-orbital ordering and Fermi surface instabilities in half-doped single-layered manganite La_0.5Sr_1.5MnO_4
D. V. Evtushinsky, D. S. Inosov, G. Urbanik, V. B. Zabolotnyy, R. Schuster, P. Sass, T. Haenke, C. Hess, B. Buechner, R. Follath, P. Reutler, A. Revcolevschi, A… 展开作者
D. V. Evtushinsky, D. S. Inosov, G. Urbanik, V. B. Zabolotnyy, R. Schuster, P. Sass, T. Haenke, C. Hess, B. Buechner, R. Follath, P. Reutler, A. Revcolevschi, A. A. Kordyuk, S. V. Borisenko
Density waves are inherent to the phase diagrams of materials that exhibit unusual, and sometimes extraordinarily useful properties, such as superconductivity and colossal magnetoresistance. While the pure charge density waves (CDW) are well described by an itinerant approach, where electrons are treated as waves propagating through the crystal, the charge-orbital ordering (COO) is usually explained by a local approach, where the electrons are treated as localized on the atomic sites. Here we show that in the half-doped manganite La0.5Sr1.5MnO4 (LSMO) the electronic susceptibility, calculated from the angle-resolved photoemission spectra (ARPES), exhibits a prominent nesting-driven peak at one quarter of the Brillouin zone diagonal, that is equal to the reciprocal lattice vector of the charge-orbital pattern. Our results demonstrate that the Fermi surface geometry determines the propensity of the system to form a COO state which, in turn, implies the applicability of the itinerant approach also to the COO.
We report inelastic neutron scattering results on the spin dynamics in the 50 % hole-doped manganites, Pr{1/2}Sr{1/2}MnO3 and Nd{1/2}Sr{1/2}MnO3. In the paramagnetic phase, these systems exhibit a ridge-type diffuse scattering, indicating a two-dimensional ferromagnetic (FM) correlation. With decreasing temperature, the systems enter the FM state, but simultaneously they develop A-type antiferromagnetic spin fluctuations. The spin wave dispersion in the FM state is strongly anisotropic. These behaviors can be consistently interpreted from a viewpoint of the underlying orbital ordering.
We observe a disappearance of electron-hole asymmetry in hole and electron doped manganites of composition Pr(1-x)Ca(x)MnO3 (x=0.36, 0.64), as reflected in the g-parameter values. The bulk property of opposite g-shifts in room temperature seems to have disappeared in nanoparticles. We analyze the results in the light of ferromagnetic fluctuations and melting of charge order in nanoparticles.
X-Ray diffraction, ac susceptibility and electrical resistivity measurements were performed in order to investigate the effect of Ag substitution for Pr in the polycrystalline Pr$_{1-x}$Ag$_x$MnO$_3$ (0.0$\leq$x$\leq$0.25) manganites. The XRD results show that the samples crystallize in the O'-orthorhombic structure with a cooperative Jahn-Teller deformation. We give evidence that the Ag$^{+}$ is not substituted at the Pr$^{3+}$ site in the PrMnO$_{3}$ structure. The increase of $T_{C}$ up to 130 K is suggested to be due to further oxidation of manganite grains by the oxygen released from the …
Using time-of-flight and triple-axis inelastic neutron spectroscopy, we determine spin wave excitations throughout the Brillouin zone for ferromagnetic manganites La$_{1-x}$Ca$_x$MnO$_3$ ($x=0.25,0.3$) in their low temperature metallic states. While spin wave excitations in the long wavelength limit (spin stiffness $D$) have similar values for both compounds, the excitations near the Brillouin zone boundary of La$_{0.7}$Ca$_{0.3}$MnO$_3$ are considerable softened in all symmetry directions compared to that of La$_{0.75}$Ca$_{0.25}$MnO$_3$. A Heisenberg model with the nearest neighbor and the f…
In order to reveal many-body interactions in the three-dimensional (3D) perovskite manganite, we have performed an $in$ $situ$ angle-resolved photoemission spectroscopy (ARPES) on La$_{0.6}$Sr$_{0.4}$MnO$_3$ (LSMO) and investigated the behaviors of quasiparticles. We observe quasiparticle peaks around the Fermi momentum, both in the electron and the hole bands, and clear kinks throughout the hole Fermi surface in the ARPES band dispersion. The isotropic behavior sharply contrasts to the strong anisotropic quasiparticle excitation observed in layered manganites. These results suggest that polar…
We investigate the high temperature phase of layered manganites, and demonstrate that the charge-orbital phase transition without magnetic order in La$_{0.5}$Sr$_{1.5}$MnO$_4$ can be understood in terms of the density wave instability. The orbital ordering is found to be induced by the nesting between segments of Fermi surface with different orbital characters. The simultaneous charge and orbital orderings are elaborated with a mean field theory. The ordered orbitals are shown to be $d_{x^2-y^2} \pm d_{3z^2-r^2}$.
We report on a high-pressure Raman study on two members of the La$_{1-x}$Ca$_x$MnO$_{3-δ}$ manganite family ($x=0.20$, $δ=0$ and $δ=0.08$). The results obtained for the $δ=0$ sample show a different behavior in the low and high pressure regimes ascribed to the onset of a new pressure-activated interaction previously invoked in other manganite compounds. The comparison of our results with literature data gives further support to the identification of the Jahn-Teller active stretching mode and shows that pressure-induced octahedral symmetrization is more effective in systems exhibiting a lower m…
We have resolved a controversial issue concerning the oxygen-isotope shift of the ferromagnetic transition temperature T_{C} in the manganite La_{0.8}Ca_{0.2}MnO_{3+y}. We show that the giant oxygen-isotope shift of T_C observed in the normal oxygen-isotope exchanged samples is indeed intrinsic, while a much smaller shift observed in the argon annealed samples is an artifact. The argon annealing causes the 18O sample to partially exchange back to the 16O isotope due to a small 16O contamination in the Ar gas. Such a contamination is commonly caused by the oxygen outgas that is trapped in the t…
The critical regime of the charge exchange (CE) manganite spin glass Eu_{0.5}Ba_{0.5}MnO_{3} is investigated using linear and non linear magnetic susceptibility and the divergence of the third ordered susceptibility (chi{_3}) signifying the onset of a conventional freezing transition is experimentally demonstrated. The divergence in chi{_3}, dynamical scaling of the linear susceptibility and relevant scaling equations are used to determine the critical exponents associated with this freezing transition, the values of which match well with the 3D Ising universality class. Magnetic field depende…
We report new zero-field muon spin relaxation and neutron spin echo measurements in ferromagnetic (FM) (La,Ca)MnO3 which taken together suggest two spatially separated regions in close proximity possessing very different Mn-ion spin dynamics. One region corresponds to an extended cluster which displays 'critical slowing down' near Tc and an increasing volume fraction below Tc. The second region possesses more slowly fluctuating spins and a decreasing volume fraction below Tc. These data are discussed in terms of the growth of small polarons into overlapping regions of correlated spins below Tc…
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$$_{0.5}$Ba$_{0.5}$MnO$_3$ was successfully synthesized and compared with $R$BaMn$_2$O$_6$ in the structures and electromagnetic properties. $R$$_{0.5}$Ba$_{0.5}$MnO$_3$ has a primitive cubic perovskite cell. Unexpectedly the magnetic glassy states are dominant as the ground state for $R$$_{0.5}$Ba$_{0.5}$MnO$_3$. A peculiar behavior, t…
The nature of the phase transitions in La$_{1-x}$Ca$_x$MnO$_3$ and Pr$_{0.48}$Ca$_{0.52}$MnO$_3$ has been probed using heat capacity and magnetisation measurements. The phase transition associated with the onset of the stripe phase has been identified as second order. The model of a Peierls transition in a disordered system (a `dirty' Peierls transition) is shown to provide an extremely good fit to this transition. In addition, an unexpected magnetic phase has been revealed in low temperature Pr$_{0.48}$Ca$_{0.52}$MnO$_3$, associated with an excess heat capacity over a wide temperature range c…
The pressure dependence of the Curie temperature T$_{C}(P)$ in La$_{0.75}$Ca$_{0.25}$MnO$_{3}$ was determined by neutron diffraction up to 8 GPa, and compared with the metallization temperature T$_{IM}(P)$ \cite{irprl}. The behavior of the two temperatures appears similar over the whole pressure range suggesting a key role of magnetic double exchange also in the pressure regime where the superexchange interaction is dominant. Coexistence of antiferromagnetic and ferromagnetic peaks at high pressure and low temperature indicates a phase separated regime which is well reproduced with a dynamical…
We address the issue of massive phase separation (PS) in manganite family of doped Mott insulators through ac conductivity measurements on La$_{0.625-y}$Pr$_{y}$Ca$_{0.375}$MnO$_{3}$ (0.375 $\leq$ y $\leq$ 0.275), and establish applicability of the scaling theory of percolation in the critical regime of the PS. Measurements of dc resistivity, magnetization (M(T)) and electron diffraction show incomplete growth of a ferromagnetic (FM) metallic component on cooling the high temperature charge ordered (CO) phase well below Curie temperature. The impedance $\mid$Z(T,f)$\mid$ measured over a freque…
We report on an a $μ$SR and $^{55}$Mn NMR investigation of the magnetic order parameter as a function of temperature in the optimally doped La$_{5/8}$(Ca$_y$Sr$_{1-y}$)$_{3/8}$MnO$_3$ and in the underdoped La$_{1-x}$Sr$_{x}$MnO$_3$ and La$_{1-x}$Ca$_{x}$MnO$_3$ metallic manganite families. The study is aimed at unraveling the effect of lattice distortions, implicitly controlled by the Ca-Sr isoelectronic substitution, from that of hole doping $x$ on the Curie temperature $T_c$ and the order of the magnetic transition. At optimal doping, the transitions are second order at all $y$ values, inclu…
We investigated slow relaxations of the magnetostriction and residual magnetostriction of the phase-separated system (Eu$_{1-x}$Gd$_{x}$)$_{0.6}$Sr$_{0.4}$MnO$_3$, in which the metamagnetic transition from a paramagnetic insulating state to a ferromagnetic metallic state is accompanied by a lattice shrinkage. The relaxations are well fitted by a stretched exponential function, suggesting the strong frustraction between the double exchange interaction and Jahn-Teller effect. We have revealed that the Gd substitution suppresses the frozen phase-separated phase at low temperatures and stabilizes …
We report on pulsed and DC I-V characteristics of polycrystalline samples of three charge-ordered manganites, Pr_{2/3}Ca_{1/3}MnO_3, Pr_{1/2}Ca_{1/2}MnO_3, Bi_{1/2}Sr_{1/2}MnO_3 and of a double-perovskite Sr_2MnReO_6, in a temperature range where their ohmic resistivity obeys the Efros-Shklovskii variable range hopping relation. For all samples, the DC I(V) exhibits at high currents negative differential resistance and hysteresis, which mask a perfectly ohmic or a moderately nonohmic conductivity obtained by pulsed measurements. This demonstrates that the widely used DC I-V measurements are us…
We report a study on the crystal growth of the hexagonal manganites $R$MnO$_3$ ($R$ = Y, Lu, Ho, Er, and Tm) by using an optical floating-zone method. It was found that high-quality single crystals of $R$ = Y, Lu, and Ho could be easily grown with essentially the same conditions as those reported in literature, that is, with an atmosphere of normal pressure Ar and oxygen mixture and a growth rate of 2--4 mm/h. However, these conditions were not feasible for growing good crystals of $R$ = Er and Tm. The chemical analysis indicated that it was due to an off-stoichiometric phenomenon in the forme…
We report direct experimental evidence of the effect of quenched random field on magnetic ordering of La_(0.5)Gd_(0.2)Sr_(0.3)MnO_(3) manganites system. We demonstrate magnetic measurements providing serious evidence to support that quenched random field of Gd divides the system in finite size clusters which undergo cluster-glass like freezing. The size or concentration of these clusters is found to be closely related to the effect of random field, which in turn is a function of applied field.
We report the observation of superstructures associated with the oxygen 2p-states in two prototypical manganites using x-ray diffraction at the oxygen K-edge. We determine the nature of the orderings and discuss our picture with respect to novel theoretical models. In the stripe order system Bi0.31 Ca0.69 MnO3, hole-doped O states are found to be orbitally ordered, at the same propagation vector as the Mn orbital ordering, but no evidence is found to support a picture of oxygen charge stripes at this periodicity. In La 7/8 Sr 1/8 MnO3, we observe a 2p charge ordering described by alternating h…
The experimental results of studying the resistivity and magnetic susceptibility are presented for the single crystal La(1-x)Sr(x)MnO(3) (x=0.15;0.175) and CaMnO(3-d). We revealed the temperature dependence of the magnetic component of activation energy of hopping conductivity (Em) in paramagnetic phase: Em=Em0(+ or -)a/T, where the "+" sign corresponds to antiferromagnetic manganite CaMnO(3-d), and the "-" sign to ferromagnetic manganites La(1-x)Sr(x)MnO(3). It has been shown that for antiferromagnetic that temperature dependence of activation energy has a maximum coinciding with a maximum of…
$La_{0.7}Ca_{0.3}MnO_3$ samples were prepared in nano- and polycrystalline forms by sol-gel and solid state reaction methods, respectively, and structurally characterized by synchrotron X-ray diffraction. The magnetic properties determined by ac susceptibility and dc magnetization measurements are discussed. The magnetocaloric effect in this nanocrystalline manganite is spread over a broader temperature interval than in the polycrystalline case. The relative cooling power of the poly- and nanocrystalline manganites is used to evaluate a possible application for magnetic cooling below room temp…
We present diffraction data on a single-layered manganite La(0.42)Sr(1.58)MnO4 with hole doping (x>0.5). Overdoped La(0.42)Sr(1.58)MnO4 exhibits a complex ordering of charges, orbitals and spins. Single crystal neutron diffraction experiments reveal three incommensurate and one commensurate order parameters to be tightly coupled. The position and the shape of the distinct superstructure scattering points to a stripe arrangement in which ferromagnetic zigzag chains are disrupted by additional Mn4+ stripes.
Among colossal magnetoresistive manganites the prototypical ferromagnetic manganite La$_{0.7}$Sr$_{0.3}$MnO$_{3}$ has a relatively small magnetoresistance, and has been long assumed to have only weak electron-lattice coupling. Here we report that La$_{0.7}$Sr$_{0.3}$MnO$_{3}$ has strong electron-phonon coupling: Our neutron and x-ray scattering experiments show strong softening and broadening of transverse acoustic phonons on heating through the Curie temperature T$_C$ = 350 K. Simultaneously, we observe two phases where metallic resistivity and polarons coexist. The ferromagnetic polaronic me…
The ferromagnetic and insulating state observed in La$_{1-x}$Ca$_{x}$MnO$_3$, 0.125$<$x$<$0.2, is characterized by structural and magnetic anomalies below T$_C$, similar to those observed in the x$_{Sr}$$\approx$1/8. A neutron scattering study of the superlattice {\bf Q$_0$}= (0,0,1+/4)$_{cub}$ peak, and of the magnetic excitations are reported in the x$_{Ca}$=0.2 sample. The occurrence of this superstructure is associated with the observation of a gap in the spin dynamics, at a {\bf q$_0$} wave-vector ({\bf q$_0$}={\bf Q$_0$}-$τ$) with the same modulus $|${\bf q$_0$}$|$ in all directions, whi…
We study the anisotropic magnetic structures exhibited by electron-doped manganites using a model which incorporates the double-exchange between orbital ly degenerate $e_{g}$ electrons and the super-exchange between $t_{2g}$ electrons with realistic values of the Hund's coupling($J_H$), the super-exchange coupling($J_{AF}$), and the bandwidth($W$). We look at the relative stabilities of the G, C and A type antiferromagnetic ph ases. In particular we find that the G-phase is stable for low electron doping as seen in experiments. We find good agreement with the experimentally observed magnetic p…
From a general model of the Mn oxides R_{1-x}A_{x}MnO_3, we derive an effective Hamiltonian in the low-energy subspace using the projection operator method, in which a novel coupling between the spin and orbital degrees of freedom is included. A phase diagram for temperature T versus doping concentration x is computed by means of Monte Carlo simulation. Our result is consistent with experimental observations in the Mn oxides with relatively wide conduction band, such as Pr_{1-x}Sr_{x} MnO_{3} and La_{1-x}Sr_{x}MnO_{3}. According to the obtained orbital ordering, we also predict that the motion…
The problem of adequate electronic model for doped manganites like La_{1-x}Sr_{x}MnO_3 remains controversial. In such a situation we argue a necessity to discuss all possible candidate states with different valent structure of manganese and oxygen atoms, as well as different valent states of octahedral MnO_{6} centers. In frames of quantum-chemical approach, crystal field and the ligand field models we address different types of MnO_6 centers, different types of d-d, and charge transfer transitions. We draw special attention to the so-called charge transfer states related to strong intra-cente…
We present the data on depolarization of polarized neutron beam and second harmonic of magnetization ($M_2$) for Nd$_{1-x}$Ba$_x$MnO$_3$ ($x$ = 0.23, the Curie temperature $T_C \approx$ 124 K; $x$ = 0.25, $T_C \approx$ 129 K) manganites. The depolarization starts to develop below $T$* $\approx$ 147 K $> T_C$ for both samples, being larger in x = 0.25 compound. This evidences the arising of a ferromagnetic (F) cluster phase below $T$* and a growth of its relative volume fraction with increasing doping concentration that agrees with the previously published results of $M_2$ study. A characterist…
We report the evolution of the Raman active A_g phonon modes in the charge-ordered manganite Pr_{0.63}Ca_{0.37}MnO_{3} as a function of temperature from 300K to 25K. Our studies reveal that the linewidths of A_g(2) and A_g(4) phonons increase as temperature decreases. This anomalous temperature dependence of phonon lineshapes, seen for the first time in charge ordered manganites, can be quantitatively understood in terms of strong spin-phonon coupling involving t_{2g} spins and A_g phonons.
THz time-domain spectroscopy was used to directly probe the low-energy (0.5--5 meV) electrodynamics of the charge-ordered manganite Pr$_{0.7}$Ca$_{0.3}$MnO$_3$. We revealed the existence of a finite peak structure around 2--3 meV well below the charge gap $\sim300$ meV. In analogy to the low-energy optical properties of the well-studied low-dimensional materials, we attributed this observed structure to the collective excitation mode arising from the charge-density-wave condensate. This finding provides the importance role of the quasi-one dimensional nature of the charge and orbital ordering …
We performed detailed ac susceptibility measurements on Pr$_{1-x}$Ag$_x$MnO$_3$ ($x$=0.15, 0.20) manganites and observed unusual and interesting features, which are associated with the domain walls and the effects of grain-boundaries on their movements. It is shown that the ac field, frequency, temperature, thermal cycling and grain coupling significantly influence the real and especially imaginary parts of the ac susceptibility. We argue that the cooperative depinning of the domain walls from the grain-boundaries accompanying with a large distance movements of the walls leads to the appearanc…
Oxygen isotope effects on the transport properties have been studied in high-quality epitaxial thin films of La_{0.75}Ca_{0.25}MnO_{3} and Nd_{0.7}Sr_{0.3}MnO_{3}. In the paramagnetic state, the resistivity can be well fitted by ρ(T) = (A/\sqrt{T})\exp(E_ρ/k_{B}T) with the parameters A and E_{a} depending strongly on the oxygen isotope mass. The resistivity below 80 K almost perfectly follows ρ= ρ_{o}+ Bω_{s}/\sinh^{2}(\hbarω_{s}/2k_{B}T) with \hbarω_{s}/k_{B} \sim 100 K. Both ρ_{o} and B increase by about 15(3)% upon raplacing $^{16}$O by $^{18}$O. The results provide quantitative constraints…
We observed a dramatic peak in the 1/f noise at the metal-insulator transition (MIT) in low-Tc manganites. This many-orders-of-magnitude noise enhancement is observed for both polycrystalline and single-crystal samples of La{5/8-y}Pr{y}Ca{3/8}MnO{3} (y=0.35-0.4) in zero magnetic field and Pr{1-x}Ca{x}MnO{3} (x=0.35-0.5) in magnetic field. This observation strongly suggests that the microscopic phase separation in the low-Tc manganites causes formation of a percolation network, and that the observed MIT is a percolation threshold.
We study theoretically the anomalous X-ray scattering as a new probe to observe the orbital orderings and excitations in perovskite manganites. The scattering matrix is given by the virtual electronic excitations from Mn $1s$ level to unoccupied Mn $4p$ level. We find that orbital dependence of the Coulomb interaction between Mn $3d$ and Mn $4p$ electrons is essential to bring about the anisotropy of the scattering factor near the K edge. The calculated results in $MnO_6$ clusters explain the forbidden reflections observed in $La_{0.5}Sr_{1.5}MnO_4$ and $LaMnO_3$. A possibility of the observat…
The magnon dispersion in the charge, orbital and spin ordered phase in La(0.5)Sr(1.5)MnO(4) has been studied by means of inelastic neutron scattering. We find an excellent agreement with a magnetic interaction model basing on the CE-type superstructure. The magnetic excitations are dominated by ferromagnetic exchange parameters revealing a nearly-one dimensional character at high energies. The nearest neighbor ferromagnetic interaction in La(0.5)Sr(1.5)MnO(4) is significantly larger than the one in the metallic ferromagnetically ordered manganites. The large ferromagnetic interaction in the ch…
We demonstrate that an A-type antiferromagnetic (AFM) state of Pr{0.5}Sr{0.5}MnO{3} exhibits a novel charge ordering which governs the transport property. This charge ordering is stripe-like, being characterized by a wave vector q ~ (0,0,0.3) with very anisotropic correlation parallel and perpendicular to the stripe direction. This charge ordering is specific to the manganites with relatively wide one-electron band width (W) which often exhibit a metallic A-type AFM state, and should be strictly distinguished from the CE-type checkerboard-like charge ordering which is commonly observed in mang…
We have investigated the specific heat and resistivity of a single crystal of Pr_{0.63}Ca_{0.37}MnO_3 around the charge ordering (CO) transition temperature, T_{CO}, in the presence of high magnetic fields (<=12T) which can melt the charge ordered state. At low magnetic fields (<=10T), the manganite transforms from a charge-disordered paramagnetic insulating (PI) state to a charge-ordered insulating (COI) state as the temperature is lowered. The COI state becomes unstable beyond a threshold magnetic field and melts to a ferromagnetic metallic phase (FMM). This occurs for T < T_{CO}. However, a…
Elastic and inelastic neutron scattering experiments have been performed in a La$_{0.94}$Sr$_{0.06}$MnO$_3$ untwinned crystal, which exhibits an antiferromagnetic canted magnetic structure with ferromagnetic layers. The elastic small q scattering exhibits a modulation with an anisotropic q-dependence. It can be pictured by ferromagnetic inhomogeneities or polarons with a platelike shape, the largest size ($\approx17Å$) and largest inter-polaron distance ($\approx$ 38$Å$) being within the ferromagnetic layers. Comparison with observations performed on Ca-doped samples, which show the growth of …
We report on the optical properties of the hole-doped manganites Nd_{0.7}Sr _{0.3}MnO_{3}, La_{0.7}Ca_{0.3}MnO_{3}, and La_{0.7}Sr_{0.3}MnO_{3}. The low-energy optical conductivity in the paramagnetic-insulating state of these materials is characterized by a broad maximum near 1 eV. This feature shifts to lower energy and grows in optical oscillator strength as the temperature is lowered into the ferromagnetic state. It remains identifiable well below Tc and transforms eventually into a Drude-like response. This optical behavior and the activated transport in the paramagnetic state of these ma…
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…
A giant low-frequency, in-plane dielectric constant, eps~10^6, for epitaxial thin films of Ca(1-x)La(x)MnO(3) (x<=0.03) was observed over a broad temperature range, 4K <= T 300K. This phenomenon is attributed to an internal barrier-layer capacitor (IBLC) structure, with insulating boundaries between semiconducting grains. The room-temperature eps increases substantially with electron (La) doping. The measured values of eps exceed those of conventional two-phase IBLC materials based on (Ba,Sr)TiO(3) as well as recently discovered CaCu(3)Ti(4)O(12) and (Li,Ti) doped NiO.
In the charge-ordered phase of strongly doped manganites La$_{1-x}$Ca$_x$MnO$_3$ ($x \geq 0.5$) absorption lines appear in the terahertz spectral range for commensurate $x$ values right below the charge-ordering temperature. They are connected to acoustic phonons that become optically active by folding of the Brillouin zone. At lower temperatures a strongly asymmetric extra absorption band develops at frequencies corresponding to the position of the lowest-energy van Hove singularity in the reduced Brillouin zone. The band is assigned to the boson peak, i.e. to the excess of lattice vibrationa…
We investigate magnetic excitations in half-doped colossal magnetoresistance manganites. In particular, we focus on spin excitations in the CE phase originally proposed by Goodenough (Phys. Rev. 100, 564 (1955)). Using a localized spin model we calculated magnons for 3D-perovskite compounds such as La$_{1-x}$M$_x$MnO$_3$, where M=Ca,Sr,Ba, and for their 2D-laminar counterparts. We compared them with predictions for the spin excitations corresponding to other phases proposed. For the laminar half-doped manganite La$_{0.5}$Sr$_{1.5}$MnO$_4$, for which magnon measurements by inelastic neutron sca…
The infrared absorption of charge density waves coupled to a magnetic background is first observed in two manganites La{1-x}Ca{x}MnO{3} with x = 0.5 and x = 0.67. In both cases a BCS-like gap 2 Delta (T), which for x=0.5 follows the hysteretic ferro-antiferromagnetic transition, fully opens at a finite T{0} < T{Neel}, with 2 Delta(T{0})/kT{c} close to 5. These results may also explain the unusual coexistence of charge ordering and ferromagnetism in La{0.5}Ca{0.5}MnO{3}.
The magnetic correlations in the charge- and orbital-ordered manganite La(0.5)Sr(1.5)MnO(4) have been studied by elastic and inelastic neutron scattering techniques. Out of the well-defined CE-type magnetic structure with the corresponding magnons a competition between CE-type and ferromagnetic fluctuations develops. Whereas ferromagnetic correlations are fully suppressed by the static CE-type order at low temperature, elastic and inelastic CE-type correlations disappear with the melting of the charge-orbital order at high temperature. In its charge-orbital disordered phase, La(0.5)Sr(1.5)MnO(…
The orbital shapes and charge disproportionations at nominal Mn$^{3+}$ and Mn$^{4+}$ sites for the charge- and orbital-ordered phases have been studied on half-doped manganites Pr(Sr$_{0.1}$Ca$_{0.9}$)$_2$Mn$_2$O$_7$ and Eu$_{0.5}$Ca$_{1.5}$MnO$_4$ with double-layer and single-layer Mn-O networks, respectively, by means of x-ray structural analyses, in comparison with Pr$_{0.5}$Ca$_{0.5}$MnO$_3$ with the pseudo cubic network. In a single-layer Eu$_{0.5}$Ca$_{1.5}$MnO$_4$ system, the ($y^2-z^2$)/($z^2-x^2$)-type orbital shape is observed, while the ($3y^2-r^2$)/($3x^2-r^2$)-type orbital shape i…
We investigate a series of manganese oxides, the La0.225Pr0.4(Ca1-xSrx)0.375MnO3 system. The x = 0 sample is a prototype compound for the study of phase separation in manganites, where ferromagnetic and charge ordered antiferromagnetic phases coexist. Replacing Ca2+ by Sr2+ gradually turns the system into a homogeneous ferromagnet. Our results show that the material structure plays a major role in the observed magnetic properties. On cooling, at temperatures below 100 K, a strong contraction of the lattice is followed by an increase in the magnetization. This is observed both through thermal e…
Spatially resolved tunneling spectroscopic studies of colossal magnetoresistive (CMR) manganite $\rm La_{0.7}Ca_{0.3}MnO_3$ (LCMO) epitaxial films on $\rm (LaAlO_3)_{0.3}(Sr_2AlTaO_6)_{0.7}$ substrate are investigated as functions of temperature, magnetic field and spin polarization by means of scanning tunneling spectroscopy. Systematic surveys of the tunneling spectra taken with Pt/Ir tips reveal spatial variations on the length scale of a few hundred nanometers in the ferromagnetic state, which may be attributed to the intrinsic heterogeneity of the manganites due to their tendency towards …
We report x-ray scattering studies of broad peaks located at a (0.5 0 0)/(0 0.5 0)-type wavevector in the paramagnetic insulating phases of La_{0.7}Ca_{0.3}MnO_{3} and Pr_{0.7}Ca_{0.3}MnO_{3}. We interpret the scattering in terms of correlated polarons and measure isotropic correlation lengths of 1-2 lattice constants in both samples. Based on the wavevector and correlation lengths, the correlated polarons are found to be consistent with CE-type bipolarons. Differences in behavior between the samples arise as they are cooled through their respective transition temperatures and become ferromagn…
We have demonstrated the effect of pressure on magnetization jump and its associated magnetostriction in Eu$_{0.58}$Sr$_{0.42}$MnO$_{3}$. The critical field lowered by the applied pressure is explained by a suppression of the metastable blocked state, which is inherent to the phase separated manganite system exhibiting the magnetic avalanche. To reduce a factor of the bad thermal coupling in the bulk sample, and to further examine the nature of the magnetization jump, we have performed the influence of pressure on the isothermal magnetization of the powder sample. There is no discrepancy in th…
Reflectivity as a function of temperature for the La$_{0.67}$Ca$_{0.33}$MnO$_{3}$ (LCMO) film has been measured across the metal-insulator phase transition. The optical properties and their temperature dependence were determined in the infrared and visible range by fits to a Drude-Lorentz model, using exact formula for the thin film optics and the measured properties of the substrate. The phonon modes were identified and verified with lattice dynamical calculations for the ideal and distorted perovskite structure of the material. The optical conductivity shows agreement with the double exchang…
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…
Atomically flat, epitaxial, and stoichiometric thin films of the electronically phase separated compound (La$_{0.5}$Pr$_{0.5}$)$_{0.67}$Ca$_{0.33}$MnO$_{3}$ were grown on as-received and treated NdGaO$_{3}$ substrates by fine tuning of oxygen pressure during deposition. Optimal thin films with step flow growth mode show superior physical properties compared to thin films grown in off-optimal oxygen pressures, {\em viz.} the highest maximum temperature coefficient of resistance, the highest peak-resistivity temperature, and reduced coercive fields. Transport, magnetization, and x-ray diffractio…
The excitation spectrum in single-layered Nd(0.33)Sr(1.67)MnO4 and Pr(0.33)Ca(1.67)MnO4 resembles the hourglass-like excitation dispersion seen in various cuprates superconductors. However, our spin-wave dispersion in Pr(0.33)Ca(1.67)MnO4, which exhibits a large correlation length of the magnetic order, showing outward-dispersing branches starting from the incommensurate zone-centres. The magnetic correlation length is identified as the decisive parameter to suppress this branches and generating an correct hourglass shape.
The dynamic magnetic properties of the distorted perovskite system La{0.7-x}Y{x}Ca{0.3}MnO{3} (0 <= x <= 0.15) have been investigated by ac-susceptibility and dc magnetization measurements, with emphasis on relaxation and aging studies. They evidence for x >= 0.10 the appearance of a metallic cluster glass phase, that develops just below the ferromagnetic transition temperature. The clusters grow with decreasing temperature down to a temperature T(f0) at which they freeze due to severe intercluster frustration. The formation of these clusters is explained by the presence of yttrium induced loc…
We use neutron scattering to investigate the doping evolution of the magnetic correlations in the single-layer manganite $\rm Pr_{\it 1-x}Ca_{\it 1+x}MnO_4$, away from the $x=0.5$ composition where the CE-type commensurate antiferromagnetic (AF) structure is stable. We find that short-range incommensurate spin correlations develop as the system is electron doped ($x<0.5$), which coexist with the CE-type AF order. This suggests that electron doping in this system induces an inhomogeneous electronic self-organization, where commensurate AF patches with $x=0.5$ are separated by electron-rich doma…
In the present work we analyze the influence of the charge-ordering on the magnetocaloric effect of Pr$_{1-x}$Ca$_x$MnO$_3$ manganites. The results for the samples with $x<$0.30 present the usual ferromagnetic behavior, peaking at the Curie temperature T$_C$. In contrast, for the samples above the onset concentration for the charge-ordering ($x\sim$0.30), an anomalous magnetic entropy change was observed below the charge-ordering temperature $T_{CO}$, persisting for lower temperatures. This effect is associated to a positive contribution to the magnetic entropy change due to charge-ordering, w…
We have investigated the magnetic and transport properties of Pr$_{0.65}$Ca$_{0.35}$MnO$_3$ and Pr$_{0.82}$Na$_{0.18}$MnO$_3$ with almost same doping level under various magnetic fields. Upon applying a field of 4 T, both compounds undergo a metamagnetic transition from antiferromagnetic (AFM) to ferromagnetic (FM) in the low temperature region. The field-induced FM state is very stable for at least 10$^5$ s even after removing the field. This irreversible FM behavior is different from the spontaneous FM ordering as well as the FM state in a reversible metamagnetic transition. We discuss this …
