The nature of the polarons in the optimally doped colossal magnetoresistive (CMR) materials La0.7Ba0.3MnO3 (LBMO) and La0.7Sr0.3MnO3 (LSMO) is studied by elastic and inelastic neutron scattering. In both materials, dynamic nanoscale polaron correlations develop abruptly in the ferromagnetic state. However, the polarons are not able to lock-in to the lattice and order, in contrast to the behavior of La0.7Ca0.3MnO3. Therefore ferromagnetic order in LBMO and LSMO survives their formation, explaining the conventional second order nature of the ferromagnetic--paramagnetic transition. Nevertheless, the results demonstrate that the fundamental mechanism of polaron formation is a universal feature of these ferromagnetic perovskite manganites.
We have studied the sub-picosecond quasiparticle dynamics in the perovskite manganite La0.7Ca0.3MnO3 and the layered manganite La1.4Sr1.6Mn2O7 using ultrafast optical spectroscopy. We found that for T > TC, initial relaxation proceeds on the time scale of several hundred femtoseconds and corresponds to the redressing of a photoexcited electron to its polaronic ground state. The temperature and dimensionality dependence of this polaron redressing time provides insight into the relationship between polaronic motion and spin dynamics on a sub-picosecond time scale. We also observe a crossover to …
We present a small-but-sizeable magnetic polaron picture where transport at high temperatures is activated while at low temperatures it is band-like. We show that both double exchange and finite bandwidth effects are important to understand colossal magnetoresistance as well as the coincidence of the metal-insulator and the ferromagnetic transitions in manganites. The magnetic transition is explained using band-like motion of the polarons.
Based on the combined model of the double exchange and the polaron, we have studied the small-to-large polaron crossover transition and explored its effects on the magnetic and transport properties in colossal magnetoresistance (CMR) manganites. We have used the variational Lang-Firsov canonical transformation, and shown that the magnetic and transport properties of both high and low $T_C$ manganites are well described in terms of a single formalism. We have reproduced the rapid resistivity drop below $T_C$, a realistic CMR ratio, and the {\it first-order-like} sharp magnetic phase transition,…
A realistic modeling of manganites should include the Coulomb repulsion between $e_g$ electrons, the Hund's rule coupling to $t_{2g}$ spins, and Jahn-Teller phonons. Solving such a model by dynamical mean field theory, we report large magnetoresistances and spectra in good agreement with experiments. The physics of the unusual, insulating-like paramagnetic phase is determined by correlated electrons which are-due to strong correlations-easily trapped as Jahn-Teller polarons.
We show that in manganites close to half-doping novel non-bipartite magnetic phases appear due to the interplay between double exchange, superexchange and orbital ordering. In considerable part of the phase diagram the groundstate has a magnetic order that is intermediate between the canonical magnetic CE-phase and a state that we identify as the recently observed Zener polaron state. The intermediate phase shows a type of charge ordering that breaks inversion symmetry and is therefore predicted to be ferroelectric.
In the colossal magnetoresistance manganites polarons have been proposed as the charge carrier state which localizes across the metal-insulator transition. The character of the polarons is still under debate. We present an assessment of measurements which identify polarons in the metallic state of La{2/3}Sr{1/3}MnO{3} (LSMO) and La{2/3}Ca{1/3}MnO{3} (LCMO) thin films. We focus on optical spectroscopy in these films which displays a pronounced resonance in the mid-infrared. The temperature dependent resonance has been previously assigned to polaron excitations. These polaronic resonances are qu…
The metal-insulator transition in manganites is strongly influenced by the concentration of holes present in the system. Based upon an orbitally degenerate Mott-Hubbard model we analyze two possible localization scenarios to account for this doping dependence: First, we rule out that the transition is initiated by a disorder-order crossover in the orbital sector, showing that its effect on charge mobility is only small. Second, we introduce the idea of orbital polarons originating from a strong polarization of orbitals in the vicinity of holes. Considering this direct coupling between charge a…
By calculating the electronic, orbital, magnetic and lattice structure of half-doped manganites we establish the central role of oxygen buckling caused by the tilting of the MnO$_6$ octahedra -- in essence a steric effect. The buckling itself does not change the Mn-Mn bonds. Instead it drives the system towards an instability where these bonds can dimerize. In presence of electron-electron interactions, this instability can fully develop and beyond a critical buckling a Zener polaron groundstate with dimerized spins, lattice and orbitals forms spontaneously, resulting in a multiferroic state.
The growth of charge ordering phenomenon in calcium doped lanthanum manganites La1-xCaxMnO3, x 0.62, 0.67 has been studied using transmission electron microscopy TEM. The diffuse intensity characteristic of short range charge ordering is observed even at room temperature. This diffuse intensity has the local intensity maxima at the incommensurate positions q. With decreasing temperature, the intensity I of super lattice charge ordered spot and the magnitude of its modulation wave vector q increases and there exists a linear relationship between I and q of super lattice charge ordered spot. Thi…
The metal-insulator transition in manganites is strongly influenced by the concentration of holes present in the system. Based upon an orbitally degenerate Mott-Hubbard model we analyze two possible localization scenarios to account for this doping dependence: First, we rule out that the transition is initiated by a disorder-order crossover in the orbital sector, showing that its effect on charge itineracy is only small. Second, we introduce the idea of orbital polarons originating from a strong polarization of orbitals in the vicinity of holes. Considering this direct coupling between charge …
Using the Lanczos method in linear chains we study the double exchange model in the low concentration limit, including an antiferromagnetic super-exchange K. In the strong coupling limit we find that the ground state contains ferromagnetic polarons whose length is very sensitive to the value of K/t. We investigate the dispersion relation, the trapping by impurities, and the interaction between these polarons. As the overlap between polarons increases, by decreasing K/t, the effective interaction between them changes from antiferromagnetic to ferromagnetic. The scaling to the thermodynamic limi…
We report a 139La NMR investigation of low-doped insulating manganite samples (LaMnO(3+y) and La(1-x)Ca(x)MnO(3+y)) as a function of temperature. A volume fraction with fast nuclear relaxations was revealed by the inhomogeneous loss of the NMR signal over a broad temperature interval. Comparison with muSR data demonstrates that the wipe out of the 139La signal is mainly due to slowly fluctuating electric field gradients. This provides strong evidence for the slow diffusion of lattice excitations, identified with Jahn-Teller small polarons.
We report measurements of the resistivity in the ferromagnetic state of epitaxial thin films of La_{1-x}Ca_{x}MnO_{3} and the low temperature specific heat of a polycrystalline La_{0.8}Ca_{0.2}MnO_{3}. The resistivity below 100 K can be well fitted by ρ- ρ_{o} = E ω_{s}/sinh^{2}(\hbar ω_{s}/2k_{B}T) with \hbar ω_{s}/k_{B} \simeq 100 K and E being a constant. Such behavior is consistent with small-polaron coherent motion which involves a relaxation due to a soft optical phonon mode. The specific heat data also suggest the existence of such a phonon mode. The present results thus provide evidenc…
We investigate the dynamical structure factor associated with lattice fluctuations in a model that approximates the manganites. It involves electrons strongly coupled to core spins, and to lattice distortions, in a weakly disordered background. This model is solved in the adiabatic limit in two dimensions via Monte Carlo, retaining all the thermal fluctuations. In the metallic phase near the polaronic crossover this approach captures the effect of thermally induced polaron formation, and their short range correlation, on the electronic spectral functions. The dynamical fluctuations of the opti…
Inspired by the strong experimental evidence for the coexistence of localized and itinerant charge carriers close to the metal-insulator transition in the ferromagnetic phase of colossal magnetoresistive manganese perovskites, for a theoretical description of the CMR transition we propose a two-phase scenario with percolative characteristics between equal-density polaron and Zener band-electron states. We find that the subtle balance between these two states with distinctly different electronic properties can be readily influenced by varying physical parameters, producing various ``colossal'' …
Understanding the coexistence of ferromagnetism and insulating behavior in manganites is an unsolved problem. We propose a localized-band model involving effective intermediate-range electron-electron (electron-hole) repulsion (attraction) generated by cooperative electron-phonon interaction. Double exchange mechanism, involving holes virtually hopping to nearest neighbors and back, produces magnetic polarons in an antiferromagnetic environment; when these magnetic polarons coalesce and percolate the system, we get a ferromagnetic insulator. Ferromagnetism gets more pronounced when the holes (…
In this work, we report an atomic scale study on the ferromagnetic insulator manganite LaMnO$_{3.12}$ using $γ-γ$ PAC spectroscopy. Data analysis reveals a nanoscopic transition from an undistorted to a Jahn-Teller-distorted local environment upon cooling. The percolation thresholds of the two local environments enclose a macroscopic structural transition (Rhombohedric-Orthorhombic). Two distinct regimes of JT-distortions were found: a high temperature regime where uncorrelated polaron clusters with severe distortions of the Mn$^{3+}$O$_{6}$ octahedra survive up to $T \approx 800 K$ and a low …
Pressure sensitivity (up to 1 GPa) of the electrical resistivity and of the ac susceptibility was measured for low electron doping levels of Ca$_{1-x}$Y$_x$MnO$_3$ (CYMO) and of Ca$_{1-x}$Sm$_x$MnO$_3$ (CSMO) ceramic samples (0.05 $\leq$ x $\leq$ 0.15). A very weak pressure dependence of the Curie temperature (T$_c$) was observed for both systems ($\sim$ 6 K GPa$^{-1}$), when compared to the hole-doped manganites of the same T$_c$ ($\sim$ 20 K GPa$^{-1}$). Our results can be interpreted within a modified Double Exchange scenario, where pressure alters the reduction of the bandwidth produced by…
In doped manganites, the strong electron-phonon coupling due to the Jahn-Teller effect localizes the conduction-band electrons as polarons. This results in polarons are carriers responsible for transport and ferromagnetic ordering rather than the bare eg electrons, and sequentially polaron exchange model is emerged for describing ferromagnetic ordering. In Pr0.7(Sr1-xCax)0.3MnO3(x=0.3-0.6) epitaxial thin films, for higher-temperature paramagnetic state and lower-temperature ferromagnetic state, both the temperature dependent transports present behaviors of small polaron; for paramagnetic-ferro…
Recent research suggests that the charge carriers in the paramagnetic state of the magnetoresistive manganites are small polarons. Here we report studies of the oxygen-isotope effects on the intrinsic resistivity and thermoelectric power in several ferromagnetic manganites. The precise measurements of these isotope effects allow us to make a quantitative data analysis. Our results do not support a simple small-polaron model, but rather provide compelling evidence for the presence of small immobile bipolarons, i.e., pairs of small polarons. Since the bipolarons in the manganites are immobile, t…
Giant oxygen isotope effects observed in colossal magnetoresistance manganites are investigated by employing the combined model of the double exchange and interacting lattice polaron mechanism. We have shown that the isotope effects on $ T_C$ in the metallic phase and $ T_{CO}$ in the charge ordered phase of manganites can be explained well in terms of the double exchange and polaron narrowing factors with reasonable physical parameters.
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 exact nature of the low temperature electronic phase of the manganite materials family, and hence the origin of their colossal magnetoresistant (CMR) effect, is still under heavy debate. By combining new photoemission and tunneling data, we show that in La{2-2x}Sr{1+2x}Mn2O7 the polaronic degrees of freedom win out across the CMR region of the phase diagram. This means that the generic ground state is that of a system in which strong electron-lattice interactions result in vanishing coherent quasi-particle spectral weight at the Fermi level for all locations in k-space. The incoherence of …
The electrical resistivity, Hall coefficient, and thermopower as functions of temperature are reported for lightly electron-doped Ca(1-x)La(x)MnO(3)(0 <= x <= 0.10). Unlike the case of hole-doped ferromagnetic manganites, the magnitude and temperature dependence of the Hall mobility for these compounds is found to be inconsistent with small-polaron theory. The transport data are better described by the Feynman polaron theory and imply intermediate coupling (alpha \~ 5.4) with a band effective mass, m*~4.3 m_0, and a polaron mass, m_p ~ 10 m_0.
In addition to mechanisms already proposed to account for the formation in manganites of a small-polaron superlattice above the Curie temperature Tc and to a metallic-like sea of large polarons below Tc, we now consider other observed colossal-resistance inducing fields, such as magnetic, electric, photon, or strain fields. We attribute the charge-ordered phase formation to the occurrence of strong dipolar binding of vibronic small polarons arising from the phonon coupling of highly polarizable two-level orbital systems. These species having associated inherent electric and magnetic off-center…
Oxygen-isotope effects on the intrinsic resistivity 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}. We found that the residual resistivity ρ_{o} increases by about 15(3)% upon replacing ^{16}O by ^{18}O. This provides strong evidence for the presence of small or intermediate-size polarons in the metallic ferromagnetic state. Furthermore, the temperature dependent part of the resistivity at low temperatures consists of an AT^{4.5} term contributed from 2-magnon scattering, and a Bω_{s}/\sinh^{2}(\hbarω_{s}/2k_{B}T) term which aris…
We study an effective one-dimensional (1D) orbital t-J model derived for strongly correlated e_g electrons in doped manganites. The ferromagnetic spin order at half filling is supported by orbital superexchange prop. to J which stabilizes orbital order with alternating x^2-y^2 and 3z^2-r^2 orbitals. In a doped system it competes with the kinetic energy prop. to t. When a single hole is doped to a half-filled chain, its motion is hindered and a localized orbital polaron is formed. An increasing doping generates either separated polarons or phase separation into hole-rich and hole-poor regions, …
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…
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…
Neutron scattering measurements on a bilayer manganite near optimal doping show that the short-range polarons correlations are completely dynamic at high T, but then freeze upon cooling to a temperature T* 310 K. This glass transition suggests that the paramagnetic/insulating state arises from an inherent orbital frustration that inhibits the formation of a long range orbital- and charge-ordered state. Upon further cooling into the ferromagnetic-metallic state (Tc=114 K), where the polarons melt, the diffuse scattering quickly develops into a propagating, transverse optic phonon.
Angle-resolved photoemission spectroscopy data for the bilayer manganite La1.2Sr1.8Mn2O7 show that, upon lowering the temperature below the Curie point, a coherent polaronic metallic groundstate emerges very rapidly with well defined quasiparticles which track remarkably well the electrical conductivity, consistent with macroscopic transport properties. Our data suggest that the mechanism leading to the insulator-to-metal transition in La1.2Sr1.8Mn2O7 can be regarded as a polaron coherence condensation process acting in concert with the Double Exchange interaction.
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 …
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…
Temperature dependent optical conductivity spectra of a La0.7Ca0.3MnO3 (LCMO) sample were measured. In the metallic regime at very low temperatures, they clearly showed two types of absorption features, i.e., a sharp Drude peak and a broad mid-infrared absorption band, which could be explained as coherent and incoherent bands of a large lattice polaron. This elementary excitation in LCMO was found to be in a strong coupling regime and to have interactions with the spin degree of freedom.
We argue that in lightly hole doped perovskite-type Mn oxides the holes (Mn$^{4+}$ sites) are surrounded by nearest neighbor Mn$^{3+}$ sites in which the occupied $3d$ orbitals have their lobes directed towards the central hole (Mn$^{4+}$) site and with spins coupled ferromagnetically to the central spin. This composite object, which can be viewed as a combined orbital-spin-lattice polaron, is accompanied by the breathing type (Mn$^{4+}$) and Jahn-Teller type (Mn$^{3+}$) local lattice distortions. We present calculations which indicate that for certain doping levels these orbital polarons may …
The interplay of the electron-phonon interaction and of the double and super exchange magnetic effects is analyzed in the $La_{1-x}Ca_xMnO_3$ perovskites with $0<x<0.5$. By using an analytical variational scheme that allows to treat the electron-phonon interaction in a fully quantum manner it is shown that in the intermediate electron-phonon coupling regime a charge density instability occurs near the metal-insulator transition, induced by either temperature or hole doping. The system segregates in antiferromagnetic or paramagnetic small polarons and ferromagnetic large polarons domains charac…
We study the Holstein-Double Exchange model in three dimensions in the presence of substitutional disorder. Using a new Monte Carlo technique we establish the phase diagram of the clean model and then focus on the effect of varying electron-phonon coupling and disorder at fixed electron density. We demonstrate how extrinsic disorder controls the interplay of lattice polaron effects and spin fluctuations and leads to widely varying regimes in transport. Our results on the disorder dependence of the ferromagnetic T_c and metal-insulator transitions bear direct comparison to data on the `optimall…
We report anisotropic resistivity measurements on a La$_{1.2}$Sr$_{1.8}$Mn$_{2}$O$_{7}$ single crystal over a temperature $T$ range from 2 to 400 K and in magnetic fields $H$ up to 14 T. For $T\geq 218$ K, the temperature dependence of the zero-field in-plane $ρ_{ab}(T)$ resistivity obeys the adiabatic small polaron hopping mechanism, while the out-of-plane $ρ_{c}(T)$ resistivity can be ascribed by an Arrhenius law with the same activation energy. Considering the magnetic character of the polarons and the close correlation between the resistivity and magnetization, we developed a model which a…
Zhao et al. [Phys. Rev. B 62, R11 949 (2000)] reported studies of the oxygen-isotope effects on the intrinsic resistivity and thermoelectric power in the paramagnetic state of several ferromagnetic manganites. The isotope effects on the intrinsic electrical transport properties are not consistent with a simple small-polaron hopping mechanism, but can be well explained by a model where there coexist immobile bipolarons and thermally-excited small polarons. Recently, Banerjee et al. [Phys. Rev. B 68, 186401 (2003)] wrote a Comment on our paper, where they misunderstood our theoretical model, err…
We have studied the low-frequency dielectric properties of the phase-separated manganite Pr0.7Ca0.3MnO3 as a function of applied magnetic field in the low temperature phase-separated state. The dielectric constant is strongly field dependent and also depends on the magnetic field history of the sample. The dielectric behavior appears to be associated with the hopping of polaronic charge carriers, and we can derive the field dependent hopping energy barrier from the frequency dependence of the dielectric constant. This analysis allows us to associate the metal-insulator transition observed in t…
Optical conductivity spectra of a cleaved ab-plane of a La_{1.2}Sr_{1.8}Mn_2O_7 single crystal exhibit a small polaron absorption band in the mid-infrared region at overall temperatures. With decreasing temperature (T) to Curie temperature (T_C), the center frequency of the small polaron band moves to a higher frequency, resulting in a gap-like feature, and that it collapses to a lower frequency below T_C. Interestingly, with decreasing T, the stretching phonon mode hardens above T_C and softens below T_C. These concurring changes of lattice and electronic structure indicate that short range p…
We discuss the particle size driven tunability of the coexistence of ferromagnetism and ferroelectricity in Pr0.67Ca0.33MnO3(PCMO) with the help of x ray diffraction, magnetization, impedance spectroscopy, and remanent polarization measurements. The remanent polarization measurements using the positive up negative down method clearly prove the existence of ferroelectricity in PCMO with phase separation between Zener polaron(ZP) ordered P21nm and disordered Pbnm structures. We also find that the ferroelectric response is enhanced in nanocrystalline samples so long as ZP ordering is not destroye…
Within a recently proposed variational approach it has been shown that, in $La_{1-x}A_xMnO_3$ perovskites with $0<x<0.5$, near the metal-insulator transition, the combined effect of the magnetic and electron-phonon interactions pushes the system toward a regime of two coexisting phases: a low electron density one made by itinerant large polarons forming ferromagnetic domains and a high electron density one made by localized small polarons giving rise to paramagnetic or antiferromagnetic domains depending on temperature. Employing the above-mentioned variational scheme, in this paper spectral a…
We explore the possibility that polaronic distortions in the paramagnetic phase of La$_{0.67}$Ca$_{0.33}$MnO$_3$ manganites persist in the ferromagnetic phase by considering the observed electrical resistivity to arise from coexisting field- and temperature-dependent polaronic and band-electron fractions. We use an effective medium approach to compute the total resistivity of the two-component system, and find that a limit with low percolation threshold explains the data rather well. To test the validity of this model, we apply it to the thermoelectric coefficient. We propose a plausible mean-…
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 report on the influence of the lattice degrees of freedom on charge, orbital and spin correlations in colossal magnetoresistance (CMR) manganites. For the weakly doped compounds we demonstrate that the electron-phonon coupling promotes the trapping of charge carriers, the disappearance of the orbital polaron pattern and the breakdown of ferromagnetism at the CMR transition. The role of different superexchange interactions is explored.
We discuss the effects of a novel polaronic disorder in the recently proposed two-fluid model for manganites. Using effective field theory as well as direct numerical simulations, we show that this disorder can have dramatic effects in terms of the transition from ferromagnetic insulator to ferromagnetic metal upon hole-doping, including an Anderson localized regime where variable range hopping may be observed.
The Zener polarons recently found in half-doped manganites are usually seen as mixed valence entities ruled by a double exchange Hamiltonian involving only correlated electrons of the metals. They can however be considered as ferrimagnetic local units if the holes are localized on the bridging oxygen atoms as implicitely suggested by recent mean-field it ab initio calculations. In the latter case, the physics is ruled by a Heisenberg Hamiltonian involving magnetic oxygen bridges. This paper shows that the spectra resulting from the resolution of both models are analytically identical. This sin…
The physics underlying the complex glassy phenomena, which accompany the formation of polarons in optimally doped manganites (ODM) is a cumbersome issue with many unexplained aspects. In this article we present $^{139}$La and $^{55}$Mn NMR in the temperature range 80K - 900K of ODM La$_{0.67}$Ca$_{0.33}$MnO$_3$. We show that local lattice distortions, established in the Paramagnetic (PM) phase for $T<700$K, induce a genuine spin-glass state, which for $T<T_c$ consolidates with the Ferromagnetic (FM) state into a single thermodynamic phase. Comparative NMR experiments on La$_{0.77}$Ca$_{0.23}$M…
The exchange interaction of polaronic carriers with localized spins leads to a ferromagnetic/paramagnetic transition in doped charge-transfer insulators with strong electron-phonon coupling. The relative strength of the exchange and electron-phonon interactions determines whether the transition is first or second order. A giant drop in the number of current carriers during the transition, which is a consequence of local bound pair (bipolaron) formation in the paramagnetic phase, is extremely sensitive to an external magnetic field. Below the critical temperature of the transition, $T_c$, the b…
We performed high pressure experiments on La(0.8)Ca(0.2-x)Sr(x)MnO(3) (LCSMO) (0<x< 0.2) ceramic samples in order to analyze the validity of the well known relation between the A mean ionic radius (<rA>) and the Curie temperature Tc of hole-doped manganites at a fixed doping level and for doping values below the 0.3 (Mn+4/Mn+3) ratio. By considering our results and collecting others from the literature, we were able to propose a phenomenological law that considers the systematic dependence of Tc with structural and electronic parameters. This law predicts fairly well the pressure sensitivity o…
An introduction is given to the many-body coherent potential approximation (CPA) for the double-exchange (DE) model and the Holstein-DE model, the latter including coupling of the electrons to local phonons as well as to local spins. It is shown how the method can treat the local spins and phonons quantum-mechanically and how it is equivalent to dynamical mean field theory in the classical limit. In the Holstein-DE model a full discussion is given of the cross-over from weak electron-phonon coupling through intermediate coupling, where small-polaron bands begin to appear, to strong coupling wh…
In a manganite film without quenched disorder, we show texturing in the form of insulating and metallic stripes above and below Curie temperature (Tc), respectively, by high resolution scanning tunneling microscopy/spectroscopy (STM/STS). The formation of these stripes involves competing orbital and charge orders, and are an outcome of overlapping electron wave-functions mediated by long-range lattice strain. Contrary to popular perception, electronically homogeneous stripe phase underlines the efficacy of the lattice strain in bringing about charge density modulation and in impeding the cross…
The hole-doped manganite La0.7Ca0.3MnO3 and the electron-doped manganite La0.7Ce0.3MnO3 undergo an insulator to metal transition at around 250 K, above which both behave as a polaronic semiconductor. We have successfully fabricated an epitaxial trilayer (La0.7Ca0.3MnO3/SrTiO3/La0.7Ce0.3MnO3), where SrTiO3 is an insulator. At room temperature, i.e. in the semiconducting regime, it exhibits asymmetric current-voltage (I-V) characteristics akin to a p-n diode. The observed asymmetry in the I-V characteristics disappears at low temperatures where both the manganite layers are metallic. To the best…
We calculate the value of the Fröhlich electron-phonon interaction in manganites, cuprates, and some other charge-transfer insulators and show that this interaction is much stronger than any relevant magnetic interaction. A polaron shift due to the Fröhlich interaction, which is about 1 eV, suggests that carriers in those systems are small (bi)polarons at all temperatures and doping levels, in agreement with the oxygen isotope effect and other data. An opposite conclusion, recently suggested in the literature, is shown to be incorrect. The frequency and temperature dependence of the optical co…
The phase diagrams of LaMnO$_3$ perovskites have been intensely studied due to the colossal magnetoresistance (CMR) exhibited by compositions around the $\frac{3}{8}^{th}$ doping level. However, phase segregation between ferromagnetic (FM) metallic and antiferromagnetic (AFM) insulating states, which itself is believed to be responsible for the colossal change in resistance under applied magnetic field, has prevented an atomistic-level understanding of the orbital ordered (OO) state at this doping level. Here, through the detailed crystallographic analysis of the phase diagram of a prototype s…
The metallic or insulating nature of the paramagnetic phase of the colossal-magnetoresistance manganites is investigated via a double exchange Hamiltonian with diagonal disorder. Mobility edge trajectory is determined with the transfer matrix method. Density of states calculations indicate that random hopping alone is not sufficient to induce Anderson localization at the Fermi level with 20-30% doping. We argue that the metal-insulator transtion is likely due to the formation of localized polarons from nonuniform extended states as the effective band width is reduced by random hoppings and ele…
The persistent proximity of insulating and metallic phases, a puzzling characterestic of manganites, is argued to arise from the self organization of the twofold degenerate e_g orbitals of Mn into localized Jahn-Teller(JT) polaronic levels and broad band states due to the large electron - JT phonon coupling present in them. We describe a new two band model with strong correlations and a dynamical mean-field theory calculation of equilibrium and transport properties. These explain the insulator metal transition and colossal magnetoresistance quantitatively, as well as other consequences of two …
We study the possibility of nanoscale phase separation in manganites in the framework of the double exchange model. The homogeneous canted state of this model is proved to be unstable toward the formation of small ferromagnetic droplets inside an antiferromagnetic insulating matrix. For the ferromagnetic polaronic state we analyze the quantum effects related to the tails of electronic wave function and a possibility of electron hopping in the antiferromagnetic background. We find that these effects lead to the formation of the threshold for the polaronic state.
