Continuum Double Exchange Model

We present a continuum model for doped manganites which consist of two species of quantum spin-1 / 2 fermions interacting with classical spin fields. The phase structure at zero temperature turns out to be considerably rich: antiferromagnetic insulator, antiferromagnetic two band conducting, canted two band conducting, canted one band conducting, and ferromagnetic one band conducting phases are identified, all of them being stable against phase separation. There are also regions in the phase diagram where phase separation occurs

Continuum Double Exchange Model

We present a continuum model for doped manganites which consist of two species of quantum spin-1 / 2 fermions interacting with classical spin fields. The phase structure at zero temperature turns out to be considerably rich: antiferromagnetic insulator, antiferromagnetic two band conducting, canted two band conducting, canted one band conducting, and ferromagnetic one band conducting phases are identified, all of them being stable against phase separation. There are also regions in the phase diagram where phase separation occurs

Phase diagram of the bosonic double-exchange model

The phase diagram of the simplest approximation to double-exchange systems, the bosonic double-exchange model with antiferromagnetic (AFM) superexchange coupling, is fully worked out by means of Monte Carlo simulations, large-N expansions, and variational mean-field calculations. We find a rich phase diagram, with no first-order phase transitions. The most surprising finding is the existence of a segmentlike ordered phase at low temperature for intermediate AFM coupling which cannot be detected in neutron-scattering experiments. This is signaled by a maximum (a cusp) in the specific heat. Below the phase transition, only short-range ordering would be found in neutron scattering. Researchers looking for a quantum critical point in manganites should be wary of this possibility. Finite-size scaling estimates of critical exponents are presented, although large scaling corrections are present in the reachable lattice sizes.

Dynamical generation of a gauge symmetry in the double-exchange model

It is shown that a bosonic formulation of the double-exchange model, one of the classical models for magnetism, generates dynamically a gauge-invariant phase in a finite region of the phase diagram. We use analytical methods, Monte Carlo simulations and finite-size scaling analysis. We study the transition line between that region and the paramagnetic phase. The numerical results show that this transition line belongs to the universality class of the antiferromagnetic RP^(2) model. The fact that one can define a universality class for the antiferromagnetic RP^(2) model, different from the one of the O(N) models, is puzzling and somehow contradicts naive expectations about universality.

Interplay between double-exchange, superexchange, and Lifshitz localization in doped manganites

Considering the disorder caused in manganites by the substitution Mn→Fe or Ga, we accomplish a systematic study of doped manganites begun in previous papers. To this end, a disordered model is formulated and solved using the variational mean-field technique. The subtle interplay between double exchange, superexchange, and disorder causes similar effects on the dependence of T_(C) on the percentage of Mn substitution in the cases considered. Yet, in La_(2/3)Ca_(1/3)Mn_(1-y)Ga_(y)O_(3) our results suggest a quantum critical point (QCP) for y ≈ 0.1–0.2, associated to the localization of the electronic states of the conduction band. In the case of La_(x)Ca_(x)Mn_(1-y)Fe_(y)O_(3) (with x = 1/3,3/8) no such QCP is expected.

Monte Carlo determination of the phase diagram of the double-exchange model

We study the phase diagram of the double exchange model, with antiferromagnetic interactions, in a cubic lattice both at zero and finite temperature. There is a rich variety of magnetic phases, combined with regions where phase separation takes place. We identify phases, intrinsic to the cubic lattice, which are stable for realistic values of the interactions and dopings. Some of these phases break chiral symmetry, leading to unusual features.

Hybrid Monte Carlo algorithm for the double exchange model

The Hybrid Monte Carlo algorithm is adapted to the simulation of a system of classical degrees of freedom coupled to non self-interacting lattices fermions. The diagonalization of the Hamiltonian matrix is avoided by introducing a path-integral formulation of the problem, in d + 1 Euclidean space–time. A perfect action formulation allows to work on the continuum Euclidean time, without need for a Trotter–Suzuki extrapolation. To demonstrate the feasibility of the method we study the Double Exchange Model in three dimensions. The complexity of the algorithm grows only as the system volume, allowing to simulate in lattices as large as 163 on a personal computer. We conclude that the second order paramagnetic–ferromagnetic phase transition of Double Exchange Materials close to half-filling belongs to the Universality Class of the three-dimensional classical Heisenberg model.

Discontinuous transitions in double-exchange materials

It is shown that the double-exchange Hamiltonian, with weak antiferromagnetic interactions, has a rich variety of first-order transitions between phases with different electronic densities and/or magnetizations. The paramagnetic-ferromagnetic transition moves towards lower temperatures, and becomes discontinuous as the relative strength of the double-exchange mechanism and antiferromagnetic coupling is changed. This trend is consistent with the observed differences between compounds with the same nominal doping, such as La_(2/3)Sr_(1/3)MnO_(3) and La_(2/3)Ca_(1/3)MnO_(3). Our results suggest that, in the low doping regime, a simple magnetic mechanism suffices to explain the main features of the phase diagram.

Variational mean-field approach to the double-exchange model

It has been recently shown that the double exchange Hamiltonian, with weak antiferromagnetic interactions, has a richer variety of first- and second-order transitions than previously anticipated, and that such transitions are consistent with the magnetic properties of manganites. Here we present a thorough discussion of the variational mean-field approach that leads to these results. We also show that the effect of the Berry phase turns out to be crucial to produce first-order paramagnetic-ferromagnetic transitions near half filling with transition temperatures compatible with the experimental situation. The computation relies on two crucial facts: the use of a mean-field ansatz that retains the complexity of a system of electrons with off-diagonal disorder, not fully taken into account by the mean-field techniques, and the small but significant antiferromagnetic superexchange interaction between the localized spins.

Polaron liquid-gas crossover at the orthorhombic-rhombohedral transition of manganites

High-resolution synchrotron x-ray powder diffraction in La(0.7)Ca(0.3)MnO(3) shows in detail a first-order structural phase transition from orthorhombic (space-group Pnma) to rhombohedral (space-group R (3) over barc) crystal structures near T(S)=710 K. Magnetic susceptibility measurements show that the rhombohedral phase strictly obeys the Curie-Weiss law as opposed to the orthorhombic phase. A concomitant change in the electrical resistivity behavior, consistent with an alteration from nonadiabatic to adiabatic small polaron hopping regimes, was also observed at T(S). The simultaneous change in transport and magnetic properties are identified as a transition from a correlated polaron liquid for TT(S), driven by the change in the crystal symmetry.

Structure and magnetism of homometallic ludwigites: Co(3)O(2)BO(3) versus Fe(3)O(2)BO(3)

We present an extensive study of the structural, magnetic, and thermodynamic properties of the oxyborate Co(3)O(2)BO(3). This is carried out through x-ray diffraction, static and dynamic magnetic susceptibilities, and specific heat experiments in single crystals in a large temperature range. The structure of Co(3)O(2)BO(3) is composed of subunits in the form of three-leg ladders where Co ions with mixed valency are located. The magnetic properties of this Co ludwigite are determined by a competition between superexchange and double-exchange interactions in the low-dimensional subunits. We discuss the observed physical properties in comparison with the only other known homometallic ludwigite, Fe(3)O(2)BO(3). The latter presents a structural distortion in the ladders and two magnetic transitions. Both features are not found in the present study of the Co ludwigite. The reason for these differences in the structural and magnetic behavior of two apparently similar compounds is discussed.

Ligand K-edge X-ray absorption spectroscopy and DFT calculations on [Fe3S4]0,+ clusters: delocalization, redox, and effect of the protein environment

Ligand K-edge XAS of an [Fe3S4]0 model complex is reported. The pre-edge can be resolved into contributions from the í2Ssulfide, í3Ssulfide, and Sthiolate ligands. The average ligand-metal bond covalencies obtained from these pre-edges are further distributed between Fe3+ and Fe2.5+ components using DFT calculations. The bridging ligand covalency in the [Fe2S2]+ subsite of the [Fe3S4]0 cluster is found to be significantly lower than its value in a reduced [Fe2S2] cluster (38% vs 61%, respectively). This lowered bridging ligand covalency reduces the superexchange coupling parameter J relative to its value in a reduced [Fe2S2]+ site (-146 cm-1 vs -360 cm-1, respectively). This decrease in J, along with estimates of the double exchange parameter B and vibronic coupling parameter ì2/k-, leads to an S ) 2 delocalized ground state in the [Fe3S4]0 cluster. The S K-edge XAS of the protein ferredoxin II (Fd II) from the D. gigas active site shows a decrease in covalency compared to the model complex, in the same oxidation state, which correlates with the number of H-bonding interactions to specific sulfur ligands present in the active site. The changes in ligand-metal bond covalencies upon redox compared with DFT calculations indicate that the redox reaction involves a two-electron change (one-electron ionization plus a spin change of a second electron) with significant electronic relaxation. The presence of the redox inactive Fe3+ center is found to decrease the barrier of the redox process in the [Fe3S4] cluster due to its strong antiferromagnetic coupling with the redox active Fe2S2 subsite.

Magnetoresistance at artificial interfaces in the itinerant SrRuO3 ferromagnet

The magnetoresistance across interfaces in the itinerant ferromagnetic oxide SrRuO3 have been studied. To define appropriately the interfaces, epitaxial thin films have been grown on bicrystalline and laser-patterned SrTiO3 substrates. Comparison is made with results obtained on similar experiments using the double-exchange ferromagnetic oxide La2/3Sr1/3MnO3. It is found that in SrRuO3, interfaces induce a substantial negative magnetoresistance, although no traces of the low-field spin tunneling magnetoresistance are found. We discuss these results on the basis of the distinct degree of spin polarization in ruthenates and manganites and the different nature of the surface magnetic layer formed at interfaces.

Magnetic and transport properties of LaMnO3+δ, La1-xCaxMnO3, La1-xCaxMn1-yFeyO3 and La1-xSrxMn1-yFeyO3

Interest to hole-doped mixed-valence manganite perovskites is connected to the ‘colossal’ magnetoresistance. This effect or huge drop of the resistivity, ρ, in external magnetic field, B, attains usually the maximum value near the ferromagnetic Curie temperature, TC. In this thesis are investigated conductivity mechanisms and magnetic properties of the manganite perovskite compounds LaMnO3+, La1-xCaxMnO3, La1-xCaxMn1-yFeyO3 and La1- xSrxMn1-yFeyO3. When the present work was started the key role of the phase separation and its influence on the properties of the colossal magnetoresistive materials were not clear. Our main results are based on temperature dependencies of the magnetoresistance and magnetothermopower, investigated in the temperature interval of 4.2 - 300 K in magnetic fields up to 10 T. The magnetization was studied in the same temperature range in weak (up to 0.1 T) magnetic fields. LaMnO3+δ is the parent compound for preparation of the hole-doped CMR materials. The dependences of such parameters as the Curie temperature, TC, the Coulomb gap, Δ, the rigid gap, γ, and the localization radius, a, on pressure, p, are observed in LaMnO3+δ. It has been established that the dependences above can be interpreted by increase of the electron bandwidth and decrease of the polaron potential well when p is increased. Generally, pressure stimulates delocalization of the electrons in LaMnO3+δ. Doping of LaMnO3 with Ca, leading to La1-xCaxMnO3, changes the Mn3+/Mn4+ ratio significantly and brings an additional disorder to the crystal lattice. Phase separation in a form of mixture of the ferromagnetic and the spin glass phases was observed and investigated in La1- xCaxMnO3 at x between 0 and 0.4. Influence of the replacement of Mn by Fe is studied in La0.7Ca0.3Mn1−yFeyO3 and La0.7Sr0.3Mn1−yFeyO3. Asymmetry of the soft Coulomb gap and of the rigid gap in the density of localized states, small shift of the centre of the gaps with respect to the Fermi level and cubic asymmetry of the density of states are obtained in La0.7Ca0.3Mn1−yFeyO3. Damping of TC with y is connected to breaking of the double-exchange interaction by doping with Fe, whereas the irreversibility and the critical behavior of the magnetic susceptibility are determined by the phase separation and the frustrated magnetic state of La0.7Sr0.3Mn1−yFeyO3.

Study of colossal magnetoresistance and pressure effects in La2/3Ca1/3MnO2 thin films /

The main purpose of this thesis is to study properties of La2/3Cai/3Mn03, both polycrystalline ceramics and thin films. This material has striking related electrical and magnetic properties. Thin films show colossal negative magnetoresistance (CMR) near transition from an insulating to a metallic state accompanied closely by transition from a paramagnetic to a ferromagnetic state. The double exchange mechanism (DE) and the Jahn-Teller deformations play an important role in CMR effect. Applied pressure has a very similar effect as does an applied magnetic field, except, at low temperatures (T