Bulk magnetization in Pr_{0.6}Ca_{0.4}MnO_3 thin films with tensile (SrTiO_3) and compressive (LaAlO_3) substrate-induced strain is compared to the magnetooptical Kerr effect (MOKE) measurements. In the absence of an external magnetic field, in both films, a stable ferromagnetic insulating majority phase coexists with an antiferromagnetic insulating phase below ~120K. MOKE measurements indicate that at 5K a metastable ferromagnetic metallic (FM) phase is formed at the surface of the stretched film in a magnetic field below 1.1T already, while in the bulk the FM phase starts to form in the field above ~4T in both films.
Due to the complex interplay of magnetic, structural, electronic, and orbital degrees of freedom, biaxial strain is known to play an essential role in the doped manganites. For coherently strained La(2/3)Ca(1/3)MnO(3) thin films grown on SrTiO(3) substrates, we measured the magnetotransport properties both parallel and perpendicular to the substrate and found an anomaly of the electrical transport properties. Whereas metallic behavior is found within the plane of biaxial strain, for transport perpendicular to this plane an insulating behavior and non-linear current-voltage characteristics (IVC…
Strained thin films of charge/orbital ordered (CO/OO) $Nd_{0.5}Ca_{0.5}MnO_3$ (NCMO) with various thickness have grown on (100)-SrTiO$_3$ and (100)-LaAlO$_3$ substrates, by using the Pulsed Laser Deposition (PLD) technique. The thickness of the films influences drastically the transport properties. As the thickness decreases, the CO transition increases while at the same time the insulator-to-metal transition temperature decreases under application of a 7T magnetic field. Clear relationships between the structural distortions and the transport properties are established. They are explained on …
We have investigated the shifts of the core-level photoemission spectra of La$_{0.6}$Sr$_{0.4}$MnO$_3$ thin films grown on three kinds of substrates, SrTiO$_3$, (LaAlO$_3$)$_{0.3}$-(SrAl$_{0.5}$Ta$_{0.5}$O$_3$)$_{0.7}$, and LaAlO$_3$. The experimental shifts of the La 4d and Sr 3d core levels are almost the same as the calculation, which we attribute to the absence of covalency effects on the Madelung potentials at these atomic sites due to the nearly ionic character of these atoms. On the other hand, the experimental shifts of the O $1s$ and Mn $2p$ core levels are negligibly small, in disagr…
We have investigated the magnetic-field-induced phase transition of charge-ordered (CO) Pr$_{0.5}$Ca$_{0.5}$MnO$_3$ thin films, deposited onto (100)-oriented LaAlO$_3$ and (100)-oriented SrTiO$_3$ substrates using the pulsed laser deposition technique, by measuring the transport properties with magnetic fields up to 22T. The transition to a metallic state is observed on both substrates by application of a critical magnetic field ($H_C>10T$ at 60K). The value of the field required to destroy the charge-ordered insulating state, lower than the bulk compound, depends on both the substrate and the…
Magnetic anisotropies of ferromagnetic thin films are induced by epitaxial strain from the substrate via strain-induced anisotropy in the orbital magnetic moment and that in the spatial distribution of spin-polarized electrons. However, the preferential orbital occupation in ferromagnetic metallic La$_{1-x}$Sr$_x$MnO$_3$ (LSMO) thin films studied by x-ray linear dichroism (XLD) has always been found out-of-plane for both tensile and compressive epitaxial strain and hence irrespective of the magnetic anisotropy. In order to resolve this mystery, we directly probed the preferential orbital occup…
With local density approximation + Hubbard $U$ (LDA+$U$) calculations, we show that the ferromagnetic (FM) insulating state observed in tensile-strained LaCoO$_3$ epitaxial thin films is most likely a mixture of low-spin (LS) and high-spin (HS) Co, namely, a HS/LS mixture state. Compared with other FM states, including the intermediate-spin (IS) state (\textit{metallic} within LDA+$U$), which consists of IS Co only, and the insulating IS/LS mixture state, the HS/LS state is the most favorable one. The FM order in HS/LS state is stabilized via the superexchange interactions between adjacent LS …
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…
At ambient pressure, bulk SrCoO$_{3}$ is a ferromagnetic (FM) metal in cubic perovskite structure. By contrast, magnetic properties of epitaxial SrCoO$_{3}$ thin films, especially at high tensile strain ($\varepsilon \gtrsim 3$\%), remain unclear: Previous calculations had predicted antiferromagnetic (AFM) states more energetically favorable in this regime, but recent experiments indicated a FM insulating state. In this work, using first-principles calculations, we perform an extensive search for the structural, spin, magnetic, and orbital states of SrCoO$_{3}$ thin films. Our calculations ind…
Measurements of the low-frequency (f<=100 kHz) permittivity and conductivity at T<= 150 K are reported for La(1-x)Ca(x)MnO(3) (0<=x<=1) and Ca(1-y)Sr(y)MnO(3) (0<=y<=0.75) having antiferromagnetic, insulating ground states covering a broad range of Mn valencies from Mn(3+) to Mn(4+). Static dielectric constants are determined from the low-T limiting behavior. With increasing T, relaxation peaks associated with charge-carrier hopping are observed in the real part of the permittivities and analyzed to determine dopant binding energies. The data are consistent with a simple model of hydrogenic im…
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…
We report the synthesis and characterization of Nd_{0.5}Sr_{0.5}MnO_{3} thin films grown by the Pulsed Laser Deposition technique on 100 -oriented LaAlO_{3} substrates. X-ray diffraction (XRD) studies show that the films are 101 -oriented, with a strained and quasi-relaxed component, the latter increasing with film thickness. We observe that transport properties are strongly dependent on the thickness of the films. Variable temperature XRD down to 100 K suggests that this is caused by substrate induced strain on the films.
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 investigate the electrical transport in mesoscopic structures of La$_{0.67}$Ca$_{0.33}$MnO$_3$ in the regime of the metal-insulator transition by fabricating microbridges from strained and unstrained thin films. We measure current-voltage characteristics as function of temperature and in high magnetic fields and with varying film thickness. For strained films, in warming from the metallic to the insulating state, we find non-linear effects in the steep part of the transition characterized by a differential resistance with a strong peak around zero applied current, and saturating at higher c…
The time resolved Magnetooptical Kerr effect in the substrate-strain-induced insulating ferromagnetic phase in (Pr$_{0.6}$Ca$_{0.4}$)MnO$_3$ thin films on two different substrates was measured in a magnetic field up to 1.1T. The photoinduced Kerr rotation and ellipticity show remarkably different magnetic-field dependence. From the comparison of the magnetic field dependencies of the photoinduced and static Kerr rotation and ellipticity we conclude that a transient ferromagnetic metallic phase, embedded within the insulating ferromagnetic phase, is created upon the photoexcitation at low tempe…
Neutron spectroscopy measurements reveal short-range spin correlations near and above the ferromagnetic-paramagnetic phase transition in manganite materials of the form La$_{1-x}A_{x}$MnO$_{3}$, including samples with an insulating ground state as well as colossal magnetoresistive samples with a metallic ground state. Quasielastic magnetic scattering is revealed that forms clear ridges running along the [100]-type directions in momentum space. A simple model consisting of a conduction electron hopping between spin polarized Mn ions that becomes self-trapped after a few hops captures the essent…
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…
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 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…
Dedicated control of oxygen vacancies is an important route to functionalizing complex oxide films. It is well-known that tensile strain significantly lowers the oxygen vacancy formation energy, whereas compressive strain plays a minor role. Thus, atomically reconstruction by extracting oxygen from a compressive-strained film is challenging. Here we report an unexpected LaCoO2.5 phase with a zigzag-like oxygen vacancy ordering through annealing a compressive-strained LaCoO3 in vacuum. The synergetic tilt and distortion of CoO5 square pyramids with large La and Co shifts are quantified using sc…
We studied the crystal and magnetic structure of the La$_{1-x}$Ca$_{x}$MnO$_{3}$ compound for $(0.11\leq x\leq 0.175)$ using stoichiometric samples. For $x<0.13$ the system's ground state is insulating canted antiferromagnetic. For $0.13\le x \le 0.175$ e below the Jahn Teller transition temperature ($T_{\rm JT}$) the crystal structure undergoes a monoclinic distortion. The crystal structure can be described with $P 2_1/c$ space group which permits two Mn sites. The unit cell strain parameter $s=2(a-c)/(a+c)$ increases for $T<T_{\rm JT}$, taking the maximum value at the Curie point, and then d…
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$), a metal-insulator transition induced by an external magnetic field is also observed and related to the collapse of the charge-ordered state. In this paper we show that the ferro-antiferromagnetic transition takes place in an inhomogeneous way: around the critical concentration the sample is a mix…
The structure, morphology, and electrical properties of epitaxial a-axis oriented thin films of Nd(0.2)Sr(0.8)MnO(3) are reported for thicknesses 10 nm <= t <= 150 nm. Films were grown with both tensile and compressive strain on various substrates. It is found that the elongated crystallographic c-axes of the films remain fully strained to the substrates for all thicknesses in both strain states. Relaxation of the a and b axes is observed for t>= 65 nm with films grown under tensile strain developing uniaxial crack arrays (running along the c axis) due to a highly anisotropic thermal expansion…
Motivated by the puzzling report of the observation of a ferromagnetic insulating state in LaMnO$_3$/SrTiO$_3$ heterostructures, we calculate the electronic and magnetic state of LaMnO$_3$, coherently matched to a SrTiO$_3$ square substrate within a "strained-bulk" geometry. We employ three different density functional theory based computational approaches: (a) density functional theory (DFT) supplemented with Hubbard U (DFT+U), (b) DFT + dynamical mean field theory (DMFT), and (c) a hybrid functional treatment of the exchange-correlation functional. While the first two approaches include loca…
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.
The valence band electronic structure of Pr$_{0.5}$Sr$_{0.5}$MnO$_3$ has been investigated across its paramagnetic metallic (PMM) - ferromagnetic metallic (FMM) - antiferromagnetic insulator (AFMI) transition. Using surface sensitive high resolution photoemission we have conclusively demonstrated the presence of a pseudogap of magnitude 80 meV in the near Fermi level electronic spectrum in the PMM and FMM phases and finite intensity at the Fermi level in the charge ordering (CO)-AFMI phase. The pseudogap behavior is explained in terms of the strong electron-phonon interaction and the formation…
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 …
The compressive strain effects on the magnetic ground state and electronic structure of strained GdTiO 3 have been studied by the first-principles method. Different from the congeneric YTiO3 and LaTiO3 cases both of which becomes the A-type antiferromagnetism on the (001) LaAlO3 substrate despite their contrastive magnetism, the ground state of strained GdTiO3 on the LaAlO3 substrate changes from the original ferromagnetism to G-type antiferromagnetim, instead of the A-type one although Gd 3+ is between Y3+ and La3+. Only when the in-plane compressive strain is large enough, e.g. on the (001) …
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 …
In this paper I report evidence that the antiferromagnetic and insulating ground state of MnO is caused by a nonadiabatic atomic-like motion as it is evidently the case in NiO. In addition, I show that the experimental findings of Goodwin et al. [Phys. Rev. Lett. (2006), 96,~047209] corroborate my suggestion that the rhombohedral-like distortion in antiferromagnetic MnO as well as in antiferromagnetic NiO is an inner distortion of the monoclinic base-centered Bravais lattice of the antiferromagnetic phases.
The effect of deposition oxygen pressure (P$_{O}$) on phase separation (PS) induced in epitaxial La$_{0.67}$Ca$_{0.33}$MnO$_{3}$/NdGaO$_{3}$(001) films was investigated. Fully oxygenated films grown at high P$_{O}$ are anisotropically strained. They exhibit PS over a wide temperature range, because of the large orthorhombicity of NdGaO$_{3}$ substrates. The paramagnetic insulator-to-ferromagnetic metal (FM) and FM-to-antiferromagnetic insulator (AFI) transitions gradually shift to lower temperatures with decreasing PO. The AFI state is initially weakened (P$_{O}$ >= 30 Pa), but then becomes mo…
We report the bulk sensitive Hard X-ray (hv=5.95keV) core level photoemission spectroscopy to investigate the intrinsic electronic structure of strained (La0.85Ba0.15)MnO3 thin films. In a 20nm thick well-strained film with strongly enhanced ferromagnetism, a new sharp satellite peak appeared at the low energy site of the Mn 2p3/2 main peak, whereas a broader signal was observed for the unstrained film with 300nm thickness. Cluster calculations revealed that the intensity corresponded to the density of the state at the Fermi level relating to the magnitude of the ferromagnetic order. The satel…
We report an infrared reflection spectroscopy study of La$_{1/2}$Ca$_{1/2}$MnO$_3$ over a broad frequency range and temperature interval which covers the transitions from the high temperature paramagnetic to ferromagnetic and, upon further cooling, to antiferromagnetic phase. The structural phase transition, accompanied by a ferromagnetic ordering at T$_C$=234 K, leads to enrichment of the phonon spectrum. A charge ordered antiferromagnetic insulating ground state develops below the Néel transition temperature T$_N$=163 K. This is evidenced by the formation of charge density waves and opening …
MnO thin films with various thicknesses and strains were grown on MgO substrates by pulsed laser deposition, then characterized using x-ray diffraction and infrared reflectance spectroscopy. Films grown on (001)-oriented MgO substrates exhibit homogenous biaxial compressive strain which increases as the film thickness is reduced. For that reason, the frequency of doubly-degenerate phonon increases with the strain, and splits below Néel temperature TN due to the magnetic-exchange interaction. Films grown on (110)-oriented MgO substrates exhibit a huge phonon splitting already at room temperatur…
We present a study of the effect of biaxial strain on the electrical and magnetic properties of thin films of manganites. We observe that manganite films grown under biaxial compressive strain exhibit island growth morphology which leads to a non-uniform distribution of the strain. Transport and magnetic properties of these films suggest the coexistence of two different phases, a metallic ferromagnet and an insulating antiferromagnet. We suggest that the high strain regions are insulating while the low strain regions are metallic. In such non-uniformly strained samples, we observe a large magn…
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…
We have studied the temperature dependence of the photoemission spectra of Pr$_{1-x}$Ca$_x$MnO$_3$ (PCMO) with $x=0.25$, 0.3 and 0.5. For $x=0.3$ and 0.5, we observed a gap in the low-temperature CE-type charge-ordered (CO) phase and a pseudogap with a finite intensity at the Fermi level ($E_F$) in the high-temperature paramagnetic insulating (PI) phase. Within the CO phase, the spectral intensity near $E_F$ gradually increased with temperature. These observations are consistent with the results of Monte Carlo simulations on a model including charge ordering and ferromagnetic fluctuations [H. …
We have measured magnetic and transport response on the polycrystalline La$_{5/8-y}$Pr$_y$Ca$_{3/8}$MnO$_3$ ($y=0.30$, average grain size 2 microns) compound. In the temperature range where ferromagnetic metallic and insulating regions coexist we observed a persistent memory of low magnetic fields ($<$ 1 T) which is determined by the actual amount of the ferromagnetic phase. The possibility to manipulate this fraction with relatively small external perturbations is related to the phase separated nature of these manganese oxide based compounds. The colossal magnetoresistance figures obtained (a…
The phase diagram of isotropically expanded graphene cannot be correctly predicted by ignoring either electron correlations, or mobile carbons, or the effect of applied stress, as was done so far. We calculate the ground state enthalpy (not just energy) of strained graphene by an accurate off-lattice Quantum Monte Carlo (QMC) correlated ansatz of great variational flexibility. Following undistorted semimetallic graphene (SEM) at low strain, multi-determinant Heitler-London correlations stabilize between $\simeq$8.5% and $\simeq$15% strain an insulating Kekule-like dimerized (DIM) state. Closer…
We investigate the ultra-sharp jump in the isothermal magnetization and the resistivity in the polycrystalline $Sm_{0.5}(Ca_{0.5-y}Sr_{y})MnO_3$ $(y = 0, 0.1, 0.2, 0.25, 0.3, 0.5)$ compounds. The critical field $(H_{cr})$, required for the ultra-sharp jump, decreases with increase of `Sr' concentration, i.e. with increase of average A-site ionic radius $\langle r_A\rangle$. The magnetotransport data indicate that the phase separation increases with the increase of $\langle r_A\rangle$, i.e. with $y$. The dependency of $H_{cr}$ with magnetic field sweep rate reveals that the ultra-sharp jump fr…
We report on DC and pulsed electric field sensitivity of the resistance of mixed valent Mn oxide based La(5/8-y)Pr(y)Ca(3/8)MnO(3) (y = 0.4) single crystals as a function of temperature. The low temperature regime of the resistivity is highly current and voltage dependent. An irreversible transition from high (HR) to a low resistivity (LR) is obtained upon the increase of the electric field up to a temperature dependent critical value (V_c). The current-voltage characteristics in the LR regime as well as the lack of a variation in the magnetization response when V_c is reached indicate the for…
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…
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 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…
We demonstrate that magnetic phase separation and competing spin order in the colossal magnetoresistive (CMR) manganites can be directly explored via tuning strain in bulk samples of nanocrystalline La$_{1-x}$Ca$_x$MnO$_3$. Our results show that strain can be reversibly frozen into the lattice in order to stabilize coexisting antiferromagnetic domains within the nominally ferromagnetic metallic state of La$_{5/8}$Ca$_{3/8}$MnO$_3$. The measurement of tunable phase separation via magnetic neutron powder diffraction presents a direct route of exploring the correlated spin properties of phase sep…
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 present the results of a study of specific heat on a single crystal of Pr$_{0.63}$Ca$_{0.37}$MnO$_3$ performed over a temperature range 3K-300K in presence of 0 and 8T magnetic fields. An estimate of the entropy and latent heat in a magnetic field at the first order charge ordering (CO) transition is presented. The total entropy change at the CO transition which is $\approx$ 1.8 J/mol K at 0T, decreases to $\sim$ 1.5 J/mol K in presence of 8T magnetic field. Our measurements enable us to estimate the latent heat $L_{CO}$ $\approx$ 235 J/mol involved in the CO transition. Since the entropy o…
A temperature-dependent EXAFS investigation of La{1-x}Ca{x}MnO3 is presented for the concentration range that spans the ferromagnetic-insulator (FMI) to ferromagnetic-metal (FMM) transition region, x = 0.16-0.22. The samples are insulating for x = 0.16-0.2 and show a metal/insulator transition for x = 0.22. All samples are ferromagnetic although the saturation magnetization for the 16% Ca sample is only ~ 70% of the expected value at 0.4T. We find that the FMI samples have similar correlations between changes in the local Mn-O distortions and the magnetization as observed previously for the co…
Sm{0.5-x}Pr{x}Sr{0.5}MnO{3} exhibits variety of ground states as x is varied from 0 to 0.5. At an intermediate doping of x = 0.3 a charge-ordered CE type antiferromagnetic insulating (AFI) ground state is seen. The transition to this ground state is from a paramagnetic insulating (PMI) phase through a ferromagnetic metallic phase (FMM). Local structures in PMI and AFI phases of x = 0.3 sample have been investigated using Pr K-edge and Sm K-edge Extended X-ray Absorption Fine Structure (EXAFS). It can be seen that the tilting and rotation of the MnO6 octahedra about the b-axis are responsible f…
The magnetic phase diagram of $La_{1-δ}MnO_{3}$ powdered samples have been studied as a function of $δ$ in the low doping range. $La_{0.97}MnO_{3}$ has a canted magnetic structure at low temperature $(θ\simeq 130\QTR{group}{{}^{\circ}})$. Above $T_{C}=118K$, it becomes a paramagnet with a huge effective magnetic moment, $μ_{eff}=6.0μ_{B}$, reflecting the presence of magnetoelastic polarons which are not affected by the magnetic field (up to 20T) nor the temperature $(1.2T_{C}<T<2.5T_{C})$. When $δ$ is increased to $δ=0.07$, polarons are still presen at high temperature, with a smaller size: $μ…
We have studied the temperature evolution of the inverse photoemission spectra of phase separated La$_{0.2}$Sr$_{0.8}$MnO$_{3}$. To identify the features in the room temperature experimental spectra, band structure calculations using Korringa-Kohn-Rostoker Green's function method were carried out. We find that the features generated by local moment disorder calculations give a better match with the experimental spectrum. In the insulating phase, we observed unusually an increased intensity at around the Fermi level. This puzzling behaviour is attributed to the shift in the chemical potential t…
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…
Transition metal oxides possess complex free energy surfaces with competing degrees of freedom. Photoexcitation allows shaping of such rich energy landscapes. In epitaxially strained $\mathrm{La_{0.67}Ca_{0.33}MnO_3}$, optical excitation with a sub-100 fs pulse above $2\ \mathrm{mJ/cm^2}$ leads to a persistent metallic phase below 100 K. Using single-shot optical and terahertz spectroscopy, we show that this phase transition is a multi-step process. We conclude that the phase transition is driven by partial charge order melting, followed by growth of the persistent metallic phase on longer tim…
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…
Ab initio calculations of the electric polarization of correlation-driven insulating materials, namely Mott insulators, have not been possible so far. Using a combination of density functional theory and dynamical-mean-field theory we study the electric polarization of the Mott insulator Sr$_{0.5}$Ba$_{0.5}$MnO$_{3}$. We predict a ferroelectric polarization of $\simeq 16.5 μC/cm^2$ in the high temperature paramagnetic phase and recover the measured value of $\simeq 13.3 μC/cm^2$ in the low temperature antiferromagnetic phase. Our calculations reveal that the driving force for the ferroelectric…
We introduce an effective model for $e_g$ electrons to describe three-dimensional perovskite (La$_{1-x}$Sr$_{x}$MnO$_3$ and La$_{1-x}$Ca$_{x}$MnO$_3$) manganites and study the magnetic and orbital order on $4\times 4\times 4$ cluster using correlated wave functions. The model includes the kinetic energy, and on-site Coulomb interactions for $e_g$ electrons, antiferromagnetic superexchange interaction between $S=3/2$ core spins, and the coupling between $e_g$ electrons and Jahn-Teller modes. The model reproduces the experimentally observed magnetic order: ($i$) $A$-type antiferromagnetic phase …
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 results of electrical resistivity, magnetoresistance and ac and dc magnetic susceptibility on polycrystalline samples of the type La(0.5)Ca(0.5-x)Ba(x)MnO(3) synthesized under identical heat treatment conditions. The substitution of larger Ba ions for Ca results in a non- monotonic variation of the curie temperature as the system evolves from a charge ordered insulating state for x=0 to a ferromagnetic metallic state for x=0.5. An intermediate compositino, x=0.1, interestingly exhibits ferromagnetic. insulating behaviour with thermal hysteresis in ac chi around the curie tem- peratu…
Magnetotransport properties of La0.7Ca0.3MnO3 thin films deposited on (100) LaAlO3 substrate were investigated. The balance between the charge ordered insulating phase and ferromagnetic metallic phase may account for a number of glassy features such as: significant hysteresis, memory effects and long-time resistivity relaxation. It was found that the resistance of La0.7Ca0.3MnO3 thin film decreases significantly upon applying electric current, in a wide temperature range 10 - 220 K. The magnetotransport properties of the strained thin films are discussed in the context of cross-coupling of cha…
