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(4) exhibits a dispersion of ferromagnetic correlations which remarkably resembles the magnon dispersion in ferromagnetically ordered metallic perovskite manganites.
Dc magnetic measurements across the charge ordering (CO) transition temperature (T$_{CO}$) in polycrystalline Pr$_{0.5}$Ca$_{0.5}$Mn$_{0.975}$Al$_{0.025}$O$_3$ have been performed under simultaneous influence of external hydrostatic pressure (P) and magnetic field (H). We show the first experimental evidence that the melting of charge order instability obey an interesting scaling function, $δ$T$_{CO}$/P$^α$ = $f$(H/P$^β$) in H-P-T landscape, where $δ$T$_{CO}$ is the suppression of T$_{CO}$ by P and H. Corresponding values of the exponents, $α$ = 1.63 and $β$ = 0.33 have been extracted from dat…
We present Raman scattering studies of the structural and magnetic phases that accompany temperature- and field-dependent melting of charge- and orbital-order (COO) in La0.5Ca0.5MnO3 and La0.25Pr0.375Ca0.375MnO3. Our results show that thermal and field-induced COO melting in La0.5Ca0.5MnO3 exhibits three stages in a heterogeneous melting process associated with a structural change: a long-range, strongly JT distorted/COO regime; a coexistence regime; and weakly JT distorted/PM or FM phase. We provide a complete structural phase diagram of La0.5Ca0.5MnO3 for the temperature and field ranges 6<=…
We investigated the temperature ($T=$ 15 $\sim $ 290 K) and the magnetic field ($H=$ 0 $\sim $ 17 T) dependent optical conductivity spectra of a charge/orbital ordered manganite, Nd$_{1/2}$Sr$_{1/2}$MnO$_3$. With variation of $T$ and $H$, large spectral weight changes were observed up to 4.0 eV. These spectral weight changes could be explained using the polaron picture. Interestingly, our results suggested that some local ordered state might remain above the charge ordering temperature, and that the charge/orbital melted state at a high magnetic field (i.e. at $H=$ 17 T and $% T=$ 4.2 K) shoul…
Superlattices built from two antiferromagnetic (AFM) charge/orbital order compounds, $Pr_{0.5}Ca_{0.5}MnO_3$ and $La_{0.5}Ca_{0.5}MnO_3$, have been studied as the thickness of $La_{0.5}Ca_{0.5}MnO_3$ ($LCMO$) varied. High structural quality thin films were obtained on $LaAlO_3$ substrates using the pulsed laser deposition technique. An antiferromagnetic-to-ferromagnetic transition, in addition to an enhancement of the coercivity, are observed as the $LCMO$ layer thickness increases. The small shift in the origin of the field-cooled hysteresis loop along the field axis indicates the presence of…
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.
The antiferromagnetic manganite Pr$_{0.5}$Sr$_{0.5}$MnO$_3$ was investigated at low temperature by means of magnetometry and $^{55}$Mn NMR. A field-induced transition to a ferromagnetic state is detected by magnetization measurements at a threshold field of a few tesla. NMR shows that the ferromagnetic phase develops from zero field by the nucleation of microscopic ferromagnetic domains, consisting of an inhomogeneous mixture of tilted and fully aligned parts. At the threshold the NMR spectrum changes discontinuously into that of a homogeneous, fully aligned, ferromagnetic state, suggesting a …
Nanowires of Pr_0.57 Ca_0.41 Ba_0.02 MnO_3 (PCBM) (diameter ~ 80-90 nm and length ~ 3.5 mm) were synthesized by a low reaction temperature hydrothermal method. Single-phase nature of the sample was confirmed by XRD experiments. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) were used to characterize the morphology and microstructures of the nanowires. While the bulk PCBM is known to exhibit charge order (CO) below 230 K along with a ferromagnetic transition at 110 K, SQUID measurements on the nanowires of PCBM show that the charge order is completely absent and a…
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.
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…
The high temperature paramagnetic state in an antiferromagnetic (AFM) insulator Pr_{1-x}Ca_{x}MnO_{3} is characterized by the ferromagnetic (FM) spin fluctuations with an anomalously small energy scale. The FM fluctuations show a precipitous decrease of the intensity at the charge ordering temperature T_{CO}, but persist below T_{CO}, and vanish at the AFM transition temperature T_{N}. These results demonstrate the importance of the spin ordering for the complete switching of the FM fluctuation in doped manganites.
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 use neutron scattering to demonstrate the presence of lattice polarons and their short-range correlations for several samples of La$_{1-x}$Ca$_x$MnO$_3$ in the Ca doping range $0.15\leq x\leq 0.3$. We establish the doping dependence of the orientation, commensuration, and coherence length of the polaron correlations and show that the populations of correlated and uncorrelated polarons are intimately related to the transport properties of the materials.
We have investigated the dielectric and magnetic properties of Eu$_{0.595}$Y$_{0.405}$MnO$_{3}$ $without$ the presence of the 4$f$ magnetic moments of the rare earth ions, and have found two ferroelectric phases with polarization along the $a$ and $c$ axes in a zero magnetic field. A magnetic field induced switching from one to the other ferroelectric phase took plase in which the direction of ferroelectric polarization changed from the a axis to the c axis by the application of magnetic fields parallel to the a axis. In contrast to the case of TbMnO$_{3}$, in which the 4$f$ moments of Tb$^{3+…
We have investigated the dielectric properties of Gd$_{1-x}$Tb$_{x}$MnO$_{3}$ crystals in magnetic fields to clarify the crossover between two distinct ferroelectric phases, GdMnO$_{3}$-type (first-order displacive) and TbMnO$_{3}$-type (second-order order-disorder). We have found that the compositional phase boundary between the phases exists around 0.3$<$$x$$<$0.4. For the $x$=0.1 sample exposed to magnetic fields above 3T, we have discovered successive ferroelectric phase transitions that occur at two different temperatures. We have determined the electric and magnetic phase diagram for $x$…
Employing a broadband microwave reflection configuration, we have measured the complex surface impedance, $Z_S(ω,T,H)$, of single crystal La$_{0.8}$Sr$_{0.2}$MnO$_3$, as a function of frequency (0.045-45 GHz), temperature (250-325 K), and magnetic field (0-1.9 kOe). The microwave surface impedance depends not only on the resistivity of the material, but also on the magnetic permeability, $\hatμ(ω,T,H)$, which gives rise to ferromagnetic resonance (FMR) and ferromagnetic anti-resonance (FMAR). The broadband nature of this experiment allows us to follow the FMR to low frequency and to deduce the…
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…
Inelastic neutron scattering experiments have been performed on single crystals of Nd$_{1-x}$Sr$_{x}$MnO$_{3}$ with x$\approx$0.5. Colossal magnetoresistance (CMR) in the manganites arises from the interplay between a ferromagnetic metallic and antiferromagnetic charge and orbital ordered insulating state. Therefore, it appears important to compare these phases concerning their underlying magnetic interaction parameters. Our investigations of the spin-wave disperion in the AFM ordered state of Nd$_{0.5}$Sr$_{0.5}$MnO$_{3}$ exhibits a strongly anisotropic stiffness. The sign of the anisotropy i…
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…
Spin, charge, and orbital structures in models for doped manganites are studied by a combination of analytic mean-field and numerical relaxation techniques. At realistic values for the electron-phonon and antiferromagnetic $t_{2g}$ spin couplings, a competition between a ferromagnetic (FM) phase and a charge-orbital ordered (COO) insulating state is found for $x$=1/4, 3/8, and 1/2, as experimentally observed in Pr$_{1-x}$Ca$_{x}$MnO$_3$ for $x$=0.3$\sim$0.5. The theoretical predictions for the spin-charge-orbital ordering pattern are compared with experiments. The FM-COO energy difference is s…
We present an inelastic light scattering study of single crystalline (La$_{1-y}$Pr$_y$)$_{1-x}$Sr$_{x}$MnO$_3$ ($0\leq x\leq0.14$,$y=0$ and $x=1/8$,$0\leq y\leq0.5$). A giant softening up to 20 - 30 cm$^{-1}$ of the Mn-O breathing mode has been observed only for the ferromagnetic insulating (FMI) samples ($0.11\leq x \leq 0.14$) upon cooling below the Curie temperature. With increasing Pr-doping the giant softening is gradually suppressed. This is attributed to a coupling of the breathing mode to orbital polarons which are present in the FMI phase.
A ferromagnetic insulating (FM-I) state in Pr0.75Ca0.25MnO3 has been studied by neutron scattering experiment and theoretical calculation. The insulating behavior is robust against an external magnetic field, and is ascribed to neither the phase separation between a ferromagnetic metallic (FM-M) phase and a non-ferromagnetic insulating one, nor the charge ordering. We found that the Jahn-Teller type lattice distortion is much weaker than PrMnO3 and the magnetic interaction is almost isotropic. These features resembles the ferromagnetic metallic state of manganites, but the spin exchange intera…
We present evidence of coexistence of electron paramagnetic resonance signal and anti-ferromagnetic resonance signals above the anti-ferromagnetic (AFM) transition ($T_N$) in $Pr_{0.5}Ca_{0.5}MnO_3$. We identify the latter with AFM rare regions within the Griffiths-like phase scenario with the associated temperature scale $T^\ast$ extending above room temperature.
Single crystalline (Bi,Ca)MnO3 (74< %Ca <82) were studied with neutron scattering, electron diffraction and bulk magnetic measurement. We discovered dynamic ferromagnetic spin correlations at high temperatures, which are replaced by antiferromagnetic spin fluctuations at a concomitant charge ordering and structural transition. Our results indicate that thermal-activated hopping of the Jahn-Teller active e_g electrons in these insulating materials, nevertheless, induce ferromagnetic interaction through double-exchange mechanism. It is the ordering of these charges competing with the double-exch…
We report low temperature specific heat measurements of Pr$_{1-x}$Ca$_{x}$MnO$_{3}$ ($0.3\leq x \leq 0.5$) and La$_{0.5}$Ca$_{0.5}$MnO$_{3}$ with and without applied magnetic field. An excess specific heat, $C^{\prime}(T)$, of non-magnetic origin associated with charge ordering is found for all the samples. A magnetic field sufficient to induce the transition from the charge-ordered state to the ferromagnetic metallic state does not completely remove the $C^{\prime}$ contribution. This suggests that the charge ordering is not completely destroyed by a "melting" magnetic field. In addition, the…
We present results of an electron paramagnetic resonance (EPR) study of Nd$_{1-x}$Sr$_x$MnO$_3$ with x = 0.5 across the paramagnetic to ferromagnetic, insulator to metal transition at 260 K (T$_c$) and the antiferromagnetic, charge ordering transition (T$_N$ = T$_{co}$) at 150 K. The results are compared with those on Nd$_{0.45}$Sr$_{0.55}$MnO$_3$ which undergoes a transition to a homogeneous A-type antiferromagnetic phase at T$_N$ = 230 K and on La$_{0.77}$Ca$_{0.23}$MnO$_3$ which undergoes a transition to coexisting ferromagnetic metallic and ferromagnetic insulating phases. For x = 0.5, the…
We report on the pressure effects on the orbital polaron lattice in the lightly doped manganites $\mathrm{La_{1-x}Sr_xMnO_{3}}$, with $x\sim 1/8$. The dependence of the orbital polaron lattice on $negative$ chemical pressure is studied by substituting Pr for La in $\mathrm{(La_{1-y}Pr_y)_{7/8}Sr_{1/8}MnO_{3}}$. In addition, we have studied its hydrostatic pressure dependence in $\mathrm{(La_{0.9}Pr_{0.1})_{7/8}Sr_{1/8}MnO_{3}}$. Our results strongly indicate that the hopping $t$ significantly contributes to the stabilization of the orbital polaron lattice and that the orbital polarons are ferr…
We have investigated the magnetic and dielectric properties of orthorhombic Eu$_{1-y}$Y$_y$MnO$_3$ ($0\leq y\leq 0.6$) single crystals without the presence of the 4$f$ magnetic moments of the rare-earth ions. In $y\geq 0.2$, the magnetic-structure driven ferroelectricity is observed. The ferroelectric transition temperature is steeply reducing with increasing $y$. In $y\geq 0.52$, two ferroelectric phases ($P\parallel a$ and $P\parallel c$) are coexistent at low temperatures. In these phases, ferroelectricity has different origin, which is evidenced by the distinctive poling-electric-field dep…
Colossal electroresistance (CER) has been observed in the ferromagnetic insulating (FMI) state of a manganite. Notably, the CER in the FMI state occurs in the absence of magnetoresistance (MR). Measurements of electroresistance (ER) and current induced resistivity switching have been performed in the ferromagnetic insulating state of a single crystal manganite of composition Nd$_0.7$Pb$_0.3$MnO$_3$ (NPMO30). The sample has a paramagnetic to ferromagnetic (Curie) transition temperature, Tc = 150 K and the ferromagnetic insulating state is realized for temperatures, T <~ 130 K. The colossal elec…
We studied the ferromagnetic topology in a Y$_{0.67}$Ca$_{0.33}$MnO$_3$ thin film with a combination of magnetic force microscopy and magnetization measurements. Our results show that the spin-glass like behavior, reported previously for this system, could be attributed to frustrated interfaces of the ferromagnetic clusters embedded in a non-ferromagnetic matrix. We found temperature dependent changes of the magnetic topology at low temperatures, which suggests a non-static Mn$^{3+}$/Mn$^{4+}$ ratio.
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…
The double-exchange model for the Mn oxides with orbital degeneracy is studied with including on-site Coulomb repulsion, Jahn-Teller (J-T) coupling and doping-induced disorder. In the strong interaction limit, it is mapped onto a single-band Anderson model, in which all scattering mechanisms can be treated on an equal footing. A sharp rise in the mean square fluctuation of lattice distortions is found near the Curie temperature $T_c$, in agreement with experiments. We show that the spin and J-T disorders lead to a metal-insulator transition (MIT) only at low carrier density. The MIT observed i…
This work reports on magnetic, dielectric, thermodynamic and magnetoelectric properties of Gd$_{1-x}$Y$_{x}$MnO$_{3}$, with 0 \leq x \leq 0.4, with emphasis on the (x, T) phase diagram, towards unraveling the role of the driving mechanisms in stabilizing both magnetic and ferroelectric orderings. The (x, T) phase diagram reflects the effect of lattice distortions induced by the substitution of $Gd^{3+}$ ion by smaller $Y^{3+}$ ion, which gradually unbalances the antiferromagnetic against the ferromagnetic exchange interactions, enabling the emergence of ferroelectricity for higher concentratio…
The resistivity in the ferromagnetic state of flux-grown La_{2/3}(Pb,Ca)_{1/3}MnO_3 single crystals, measured in magnetic fields up to 7 T, reveals a strong quadratic temperature dependence at and above 50 K. At lower temperatures, this contribution drops precipitously leaving the resistivity essentially temperature independent below 20 K. The Seebeck coefficient also reflects a change of regime at the same temperature. We attribute this behavior to a cut-off of single magnon scattering processes at long wavelengths due to the polarized bands of a double-exchange ferromagnet.
In the series La_{2/3-x}Tb_{x}Ca_{1/3}MnO_{3}, it is known that the compositions are ferromagnetic for smaller values of x and show spin glass characteristics at larger values of x. Our studies on the magnetic properties of various compositions in the La_{2/3-x}Tb_{x}Ca_{1/3}MnO_{3} series show that the cross over from ferromagnetic to spin glass region takes place above x ~ 1/8. Also, a low temperature anomaly at 30 K, observed in the ac susceptibility curves, disappears for compositions above this critical value of x. A mixed phase region coexists in the narrow compositional range 0.1 <= x <…
We have studied the influence of antiferromagnetic ordering on the local dielectric moments of the MnO_5 and LuO_7 polyhedra by measuring neutron powder diffraction patterns of LuMnO_3 at temperatures near T_N. We show that the coupling is weak, because the magnetic exchange coupling is predominantly in the ab-plane of the MnO_5 trigonal bipyramids, and the electric dipole moments, originating in the LuO_7 polyhedra, are oriented along the hexagonal c-axis. Anomalies in the dielectric properties near T_N are thus caused by the geometric constraints between the MnO_5 and the LuO_7 polyhedra.
Magnetic textures in the ferromagnetic phases of La$_{1-x}$Sr$_x$MnO$_3$ for 0.15 $< x <$ 0.30 have been investigated by Lorentz microscopy combined with small-angle electron diffraction experiments. Various types of magnetic textures characterized by stripe, plate-shaped, and cylindrical (magnetic bubble) domains were found. Two distinct types of magnetic stripe domains appeared in the orthorhombic structure with an inversion symmetry of La$_{0.825}$Sr$_{0.175}$MnO$_3$, depending significantly on magnetocrystalline anisotropy. Based on in-situ observations as functions of temperature and the …
We present magnetization studies in a series of phase separated La$_{0.5}$Ca$%_{0.5}$MnO$_{3}$ samples, with different low temperature fractions of the ferromagnetic (FM) and charge ordered-antiferromagnetic (CO-AFM) phases. A particular experimental procedure probes the effect of the magnetic field applied while cooling the samples, which promotes FM fraction enlargement and enhances the melting of the CO phase. The response of the system depending on its magnetic field history indicates the existence of three different regimes in the phase separated state which develops below T$_{C}$. Our da…
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 …
Temperature and current dependences of resistivity of bulk La$_{0.75}$Ca$_{0.25}$MnO$_{3}$ sample grown by the floating-zone method were studied using single ramp pulses of current. It is found that near the Curie temperature $T_C$ the sample resistance depends substantially on current magnitude. The observed features can be determined by inhomogeneous Joule overheating due to mixed phase state of manganites near the ferromagnetic-paramagnetic transition and percolation character of this transition.
We have investigated the role of the 4$f$ moment on the magnetoelectric (ME) effect of orthorhombic $R$MnO$_{3}$ ($R$=rare earth ions). In order to clarify the role of the 4$f$ moment, we prepared three samples: (Eu,Y)MnO$_{3}$ without the 4$f$ moment, TbMnO$_{3}$ with the anisotropic 4$f$ moment, and (Gd,Y)MnO$_{3}$ with the isotropic 4$f$ moment. The ferroelectric behaviors of these samples are different from each other in a zero magnetic field. (Eu,Y)MnO$_{3}$ and (Gd,Y)MnO$_{3}$ show the ferroelectric polarization along the a axis in the ground state, while TbMnO$_{3}$ shows it along the c…
In this article a detailed study of La$_{1-x}$Ca$_x$MnO$_3$ ($0\leq x \leq 0.23$) phase diagram using powder x-ray diffraction and magnetization measurements is presented. Unfortunately, in the related literature no properly characterized samples have been used, with consequence the smearing of the real physics in this complicated system. As the present results reveal, there are two families of samples. The first family concerns samples prepared in atmosphere ($P({\rm O}_2)=0.2$ Atm) which are all ferromagnetic with Curie temperature rising with $x$. The second family concerns samples, where a…
The ground state properties of a frustrated spin-1/2 system is studied on a trellis ladder which is composed of two zigzag ladders interacting through rung interactions. The presence of rung interaction between the zigzag ladders induces a non-magnetic ground state, although, each of zigzag ladders has ferromagnetic order in weak antiferromagnetic leg interaction limit. The rung interaction also generates rung dimers and opens spin gap which increases rapidly with rung interaction strength. The correlation between spins decreases exponentially with the distance between them.
We present resonant soft X-ray scattering (RSXS) results from small band width manganites (Pr,Ca)MnO$_3$, which show that the CE-type spin ordering (SO) at the phase boundary is stabilized only below the canted antiferromagnetic transition temperature and enhanced by ferromagnetism in the macroscopically insulating state (FM-I). Our results reveal the fragility of the CE-type ordering that underpins the colossal magnetoresistance (CMR) effect in this system, as well as an unexpected cooperative interplay between FM-I and CE-type SO which is in contrast to the competitive interplay between the …
A lightly doped perovskite mangantite La_{0.88}Sr_{0.12}MnO_3 exhibits a phase transition at T_{OO}=145 K from a ferromagnetic metal (T_C=172 K) to a novel ferromagnetic insulator.We identify that the key parameter in the transition is the orbital degree of freedom in e_g electrons. By utilizing the resonant x-ray scattering technique, orbital ordering is directly detected below T_{OO}, in spite of a significant diminution of the cooperative Jahn-Teller distortion. The new experimental features are well described by a theory treating the orbital degree of freedom under strong electron correlat…
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…
At crystalline interfaces where a valence mismatch exists, electronic and structural interactions may occur to relieve the polar mismatch leading to the stabilization of non-bulklike phases. We show that spontaneous reconstructions at polar $La_{0.7}Sr_{0.3}MnO_3$ interfaces are correlated with suppressed ferromagnetism for film thicknesses on the order of a unit cell. We investigate the structural and magnetic properties of valence-matched $La_{0.7}Sr_{0.3}CrO_3$ - $La_{0.7}Sr_{0.3}MnO_3$ interfaces using a combination of high-resolution electron microscopy, first principles theory, synchrotr…
We present evidence for the coexistence of ferromagnetic metallic and charge ordered insulating phases in strained thin films of La$_{0.67}$Ca$_{0.33}$MnO$_3$ at low temperatures. Such a phase separated state is confirmed using low temperature magnetic force microscopy and magnetotransport measurements. This phase separated state is not observed in the bulk form of this compound and is caused by the structural inhomogeneities due to the non-uniform distribution of strain in the film. The strain weakens the low temperature ferromagnetic metallic state and a charge ordered insulator is formed at…
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 report measurements and analysis of the magnetic critical phenomena in a single crystal of La${_{0.875}}$Sr${_{0.125}}$MnO${_3}$. The critical exponents associated with the ferromagnetic transition have been determined from ac susceptibility and dc magnetisation data. Techniques like the Kouvel$-$Fischer plots, modified Arrots Plots and the critical isotherm analysis were used for this purpose. The values of the the exponents $γ$, $β$ and $δ$ obtained are found to match very well with those predicted for the 3D Heisenberg model. Our results are consistent with recent numerical calculations …
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…
Metallic transition-metal oxides undergo a metal-to-insulator transition (MIT) as the film thickness decreases across a ritical thickness of several monolayers (MLs), but its driving mechanism remains controversial. We have studied the thickness-dependent MIT of the ferromagnetic metal La$_{0.6}$Sr$_{0.4}$MnO$_3$ by x-ray absorption spectroscopy and x-ray magnetic circular dichroism. As the film thickness was decreased across the critical thickness of the MIT (6-8 ML), a gradual decrease of the ferromagnetic signals and a concomitant increase of paramagnetic signals were observed, while the Mn…
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…
Neutron Brillouin scattering (NBS) method was developed using a pulsed spallation neutron source, and the feasibility of NBS was demonstrated by observing ferromagnetic spin waves in La$_{0.8}$Sr$_{0.2}$MnO$_3$ and SrRuO$_3$ powders. Gapless spin-wave excitations were observed in La$_{0.8}$Sr$_{0.2}$MnO$_3$, which were continuously extended to the lower scattering vector $Q$ from previous results using single crystals. The novel result is a well-defined quadratic $Q$ dependence in the spin-wave dispersion curve with a large energy gap in SrRuO$_3$ indicating robust spin-orbit coupling.
Monolayer MnO$_2$ is one of the few predicted two-dimensional (2D) ferromagnets that has been experimentally synthesized and is commercially available. The Mermin-Wagner theorem states that magnetic order in a 2D material cannot persist unless magnetic anisotropy (MA) is present and perpendicular to the plane, which permits a finite critical temperature. Previous computational studies have predicted the magnetic ordering and Curie temperature of 2D MnO$_2$ with DFT+U (Density Funtional Theory + Hubbard U correction), with the results having a strong dependence on the Hubbard U parameter. Diffu…
Strained Pr$_{0.5}$Ca$_{0.5}$MnO$_3$/La$_{0.5}$Ca$_{0.5}$MnO$_3$/Pr$_{0.5}$Ca$_{0.5}$MnO $_3$ trilayers were grown on (001)-SrTiO$_3$ substrates using the pulsed-laser deposition technique. The coupling at the interfaces of several trilayers has been investigated from magnetization and electronic transport experiments. An increase of La$_{0.5}$Ca$_{0.5}$MnO$_3$ layer thickness induces a magnetic ordering in the strain layers and at the interfaces leading to ferromagnetic behavior and enhanced coercivity, while resistivity shows metal-like behaviors. These effects are not observed in the parent…
The low temperature behavior of Pr$_{1-x}$Ca$_{x}$MnO$_{3}$ manganites are known to undergo a transition at $x\sim$0.3, from an insulating ferromagnetic state, at low Ca concentration, to an insulating antiferromagnetic state. Above the onset concentration for the charge-ordering effect ($x\sim 0.3$), a metal-insulator transition induced by an external magnetic field is also observed and related to the collapse of the charge-ordered state. In this paper we show that the ferro-antiferromagnetic transition takes place in an inhomogeneous way: around the critical concentration the sample is a mix…
Recent progress in the field of multiferroics led to the discovery of many new materials in which ferroelectricity is induced by cycloidal spiral orders. The direction of the electric polarization is typically constrained by spin anisotropies and magnetic field. Here, we report that the mixed rare-earth manganite, Gd$_{0.5}$Dy$_{0.5}$MnO$_3$, exhibits a spontaneous electric polarization along a general direction in the crystallographic ac-plane, which is suppressed below 10 K but re-emerges in an applied magnetic field. Neutron diffraction measurements show that the polarization direction resu…
Using neutron reflectometry and resonant x-ray techniques we studied the magnetic proximity effect (MPE) in superlattices composed of superconducting YBa$_2$Cu$_3$O$_7$ (YBCO) and ferromagnetic-metallic (FM-M) La$_{0.67}$Ca$_{0.33}$MnO$_{3}$ (LCMO) or ferromagnetic-insulating (FM-I) LaMnO$_{3+δ}$ (LMO). We find that the MPE strongly depends on the electronic state of the manganite layers, being pronounced for the FM-M LCMO and almost absent for FM-I LMO. We also detail the change of the magnetic depth profile due to the MPE and provide evidence for its intrinsic nature.
We studied the charge-orbital ordering in the superlattice of charge-ordered insulating Pr$_{0.5}$Ca$_{0.5}$MnO$_3$ and ferromagnetic metallic La$_{0.5}$Sr$_{0.5}$MnO$_3$ by resonant soft x-ray diffraction. A temperature-dependent incommensurability is found in the orbital order. In addition, a large hysteresis is observed that is caused by phase competition between insulating charge ordered and metallic ferromagnetic states. No magnetic phase transitions are observed in contrast to bulk, confirming the unique character of the superlattice. The deviation from the commensurate orbital order can…
