Room-temperature phase separation in weakly doped lanthanum manganites

The properties of single crystals of weakly doped lanthanum manganites La_1?xA_xMnO₃ (A = Ca, Ce, Sr; x = 0, 0.07?0.1) have been studied in the temperature range from 77 to 400 K. It is established that these lanthanum manganites exhibit (in addition to the well-known characteristic features observed in the region of the temperature of magnetic ordering) changes in the electrical and magnetic properties in the region of room temperature (T ≈ 270–300 K), which is about two times the Curie temperature (T ≈ 120–140 K) and is far from the temperature of structural transitions in the samples studied. The results are explained in terms of phase separation related to the formation of magnetic clusters in the nonconducting medium. The phase separation is caused by a gain in the exchange energy and by the development of elastic stresses in the crystal lattice and proceeds via combination of small-radius magnetic polarons into a large-size magnetic cluster containing several charge carriers. The short-range order in the cluster appears and the phase separation begins at a temperature T_ps, which is close to T_C ≈ 300 K, typical of doped conducting manganites. The results of magnetic measurements show that, as the temperature decreases from 300 to 190 K, the size of superparamagnetic droplets increases from about 8 to 15 Å.     

掺杂锰基氧化物中的相分离和渗流效应

目前，相分离仍是锰基氧化物超大磁电阻材料研究的热点，渗流效应假设已广泛用于解释其电输运特性．作者用变温磁力显微镜首次在La0.33Pr0.34Ca0.33MnO3薄膜中直接观察到了渗流过程，微观上证明了渗流效应假设的正确性．实验发现，降温过程中电阻率的陡降是铁磁金属相的渗流效应引起的，升温过程中电阻率的上升，则是由导电路径上磁畴的磁化强度随温度的升高而降低引起的，而导电路径一直存在．微观的磁回滞和宏观的电阻回滞相吻合．当然要定量解释锰氧化物中的超大磁电阻效应还需要做大量的理论和实验工作．     

Theory of insulator metal transition and colossal magnetoresistance in doped manganites

The persistent proximity of insulating and metallic phases, a puzzling characteristic 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 state coexistence.     

Origin of the electron spin resonance signal in the manganites: from polarons to phase separation

In the manganites L_1?xM_xMnO₃ (L = La, Nd, Pr, …; M = Sr, Ba, Ca, …), the doping concentration introduces a mixed valence (Mn³⁺, Mn⁴⁺) which governs the magnetic and electric properties of the compound. Mn³⁺ (S = 2) is scarcely observed in electron spin resonance (ESR). In contrast, Mn⁴⁺ (S = 3/2), is a good ESR probe. However, X-band measurements show an enhanced Mn⁴⁺ susceptibility, which is the signature of some kind of coupling of the Mn⁴⁺ ions with the Mn³⁺ ions, but its exact nature is still controversial. We present multifrequency ESR experiments (9–385 GHz) obtained on different systems (La_1?δMnO₃, La_1?xMnO₃, La_1?xCa_xMnO₃, and Nd_1?xCa_xMnO₃) in the low-concentration range (0 <x< 0.33). In the paramagnetic regime, the Mn³⁺ spectrum cannot be observed because of fast relaxation. The signal arises from polarons, whose size, temperature and magnetic field dependences vary with M andx. The single line observed in the metallic compound evolves towards a double-peak structure visible at high frequency in La_0.97MnO₃. Its evolution with temperature below the magnetic transition reveals the presence of manganese ions in a different magnetic environment, i.e., phase separation. The magnetic order of the separated phase is not ferromagnetic. It is a more complex order, which depends substantially on the nature of the cation M.     

Curie temperature and frustrated phase separation in manganites

There is an increasing experimental evidence that phase separation between insulating and metallic phase plays an important role in the physics of manganites. On general grounds one can argue that the electronic density in the metallic and insulating region will be generally different. This implies that phase separation of the ordinary “Maxwell construction” type is frustrated by the long-range Coulomb interaction. We present a generalization of Maxwell construction to this situation. The system is assumed to separate in islands of one phases hosted by the other. The size of the islands is determined minimizing a free energy that takes into account both surface energy and Coulomb effects. We discuss the peculiarities of this kind of phase separation and the consequences for the manganites. In particular, we present an explanation for the non-monotonous behavior of the Curie temperature as a function of doping.     

Interplay of charge, spin, orbital and lattice correlations in colossal magnetoresistance manganites

We derive a realistic microscopic model for doped colossal magnetoresistance manganites, which includes the dynamics of charge, spin, orbital and lattice degrees of freedom on a quantum mechanical level. The model respects the SU(2) spin symmetry and the full multiplet structure of the manganese ions within the cubic lattice. Concentrating on the hole doped domain ( 0≤x≤0.5) we study the influence of the electron-lattice interaction on spin and orbital correlations by means of exact diagonalisation techniques. We find that the lattice can cause a considerable suppression of the coupling between spin and orbital degrees of freedom and show how changes in the magnetic correlations are reflected in dynamic phonon correlations. In addition, our calculation gives detailed insights into orbital correlations and demonstrates the possibility of complex orbital states. Received 4 September 2002 / Received in final form 8 November 2002 Published online 31 December 2002     

Magnetic-field-controlled phase separation in manganites: Electron magnetic resonance study

The electron magnetic resonance spectra of Sm_1?x Sr _x MnO₃ (x = 0.30, 0.40, 0.45) manganites have been studied. At temperatures that are higher than the Curie point by several tens of kelvins, samples with x = 0.40 and 0.45 exhibit a ferromagnetic resonance (FMR) spectrum imposed on their usual EPR spectrum. The FMR spectrum appears as the applied magnetic field H exceeds a certain critical field H _c , which decreases upon cooling and becomes zero at T = T _C . These results agree with the magnetic-measurement data and indicate the magnetic-field-induced nucleation and growth of ferromagnetic domains in a paramagnetic matrix. In the initial growth stage, the volume of the ferromagnetic domains is proportional to (H ? H _c )^β, where β = 4.0 ± 0.3, and it changes in phase with magnetic field modulation up to a frequency of 100 kHz. In the same field and temperature ranges, hysteretic phenomena and narrow unstable spectral lines are detected; these lines indicate a dynamic character of the phase separation. The results obtained are interpreted in terms of the competition of different types of magnetic and charge ordering.     

Non-linear spin fluctuations and phase transitions in itinerant electron magnets: CMR manganites

We present a review analyzing the effects of coupling of transverse magnons with longitudinal spin fluctuations in isotropic itinerant ferro- and antiferromagnets. It is shown that this coupling essentially changes the spectrum of longitudinal fluctuations. At low-temperatures their spectrum is dominated by the linear Landau relaxation, is purely quasielastic and described by a broad central peak of a paramagnon type. On approaching the critical temperature non-linear magnetic relaxation due to mode–mode couplings can dominate and lead to a rapid increase of the central peak and to a new mechanism of magnetic phase transitions governed by non-linear spin fluctuations. The formalism is applied to the CMR manganites where the observed quasielastic fluctuations can be viewed as non-linear spin-lattice fluctuations strongly affected by magnons.     

Phase separation and anisotropy in the electrical properties of weakly doped lanthanum manganites

Variations in the thermopower, electrical resistivity, magnetoresistance, thermal expansion coefficients, and their anisotropy with temperature were detected near room temperature in single crystals of weakly doped lanthanum manganites La_1?xA_xMnO₃ (A = Ca, Sr; x = 0.07–0.125) with orthorhombic structure. The results obtained are discussed in terms of a model of phase separation related to polaron anisotropy. Due to a gain in exchange and elastic energies in the lattice, small-radius magnetic polarons can merge to form polarons of a larger size, which would contain now not one but rather a few electrons (equal in number to the polarons in the cluster). As a result, short-range order in a cluster and phase separation set in at a temperature T_ps ≈ 250–300 K, which is approximately equal to the Curie temperature T_C of conducting manganites with x ≈ 0.2–0.3.     

Interrelation of the magnetic structure and the band insulating state in doped manganites

The interrelation between the magnetic structure and the band insulating state in doped La_{1 − x} Ca _x MnO₃ manganites has been discussed. An analysis of various zigzag chains has revealed that, in the one-dimensional spectrum of e _g electrons of these compounds, there always appear a number of band gaps, which at certain electron concentrations x support the formation of an insulating state in the corresponding three-dimensional antiferromagnetic structures. Apart from the well-known spectra of chains of the type (1 × 1) (magnetic E-structure) and (2 × 2) (magnetic CE-structure), we have obtained for the first time the spectrum of a (3 × 3) zigzag chain, whose three-dimensional unit cell contains 24 manganese atoms and provides a qualitatively correct fit to the magnetic structure of the La_1/3Ca_2/3MnO₃ manganite. As follows from our analysis, the formation of a magnetic structure in this manganite should also be accompanied by the generation of a spontaneous magnetic moment.     

Study of doping effect,phase separation and heterojunction in CMR manganites

Mixed-valence manganites have attracted considerable research focus in recent years not only because of the potential application of colossal magnetoresistance(CMR) in magnetic devices,but also because of many intriguing physical properties observed in these materials.Doping elements at A-site can alter the filling of 3d Mn band and the tolerance factor.Therefore the hole-and electron-doped CMR manganites exhibit a rich phase diagram.In addition,more theoretical and experimental results suggest that phase separation is a critical factor for the understanding of CMR phenomena.Recently,there is an increasing interest in the fabrication and investigation on manganite-based heterojunction,which demonstrated excellent rectifying property,large MR,and photovoltaic effect.     

Ground state degeneracy and ferromagnetism in a spin glass

We prove three results for the two-dimensional Ising spin glass model on a square lattice: (a) finite entropy for the ground state; (b) ferromagnetism for low concentrations of antiferromagnetic bonds and low temperatures; (c) vanishing magnetization for a spin glass with equal concentrations of ferro- and antiferromagnetic bonds.     

相分离Nd0.5Ca0.5MnO3体系的再入型自旋玻璃行为和电荷有序

K左右出现典型再入型自旋玻璃行为,同时观察到了负的磁化率异常. 结果表明,Nd0.5Ca0.5MnO3体系在低温下存在着典型的相分离和多种复杂的磁相互作用竞争机制,这为强关联锰氧化物体系物理机制的理解提供了重要的实验资料.     

Orbital and spin effects in the low-temperature behavior of the magnetoresistance of doped CdTe crystals

An observation of the suppression of negative magnetoresistance in samples of doped CdTe that are far from the metal-insulator transition as the temperature is lowered in the temperature range 3–0.4 K was previously reported [N. V. Agrinskaya, V. I. Kozub, and D. V. Shamshur, JETP 80, 1142 (1995)]. The results of an investigation of samples that are closer to the transition in the low-temperature region below 36 mK are presented. It is discovered that the samples investigated (which do not exhibit the suppression of negative magnetoresistance at comparatively high temperatures) display this effect at low temperatures and that, as previously, the suppression of the negative magnetoresistance correlates with the transition to conduction via Coulomb-gap states. A plateau-like magnetoresistance feature is displayed at low temperatures for the sample that is closest to the metal-insulator transition. The results obtained are analyzed within existing theoretical models that take into account the role of both the orbital and spin degrees of freedom. In particular, the low-temperature feature indicated is interpreted as a manifestation of positive magnetoresistance caused by spin effects. Nevertheless, it is shown within a detailed analysis supplemented by numerical calculations that the observed suppression of the negative magnetoresistance cannot be attributed only to the appearance of spin positive magnetoresistance. Moreover, the possibility of observing spin positive magnetoresistance is determined to a certain extent specifically by the suppression of the negative magnetoresistance competing with it. Zh. éksp. Teor. Fiz. 111, 1477–1493 (April 1997)     

Understanding the insulating phase in colossal magnetoresistance manganites: shortening of the Jahn-Teller long-bond across the phase diagram of La1-xCaxMnO3

The detailed evolution of the magnitude of the local Jahn-Teller (JT) distortion in La(1-x)Ca(x)MnO3 is obtained across the phase diagram for 0< or =x< or =0.5 from high-quality neutron diffraction data using the atomic pair distribution function method. A local JT distortion is observed in the insulating phase for all Ca concentrations studied. However, in contrast with earlier local structure studies, its magnitude is not constant, but decreases continuously with increasing Ca content. This observation is at odds with a simple small-polaron picture for the insulating state.     

Heat capacity and magnetoresistance of a lightly doped two-dimensional antiferromagnet in the noncollinear phase

The energy spectrum of mobile charge carriers in a two-dimensional Antiferromagnet placed in external magnetic field is analyzed. It is shown that allowing for the magnetic sublattice skew the effective mass of mobile charge carriers in a lightly doped Antiferromagnet. This affects substantially the transport and thermodynamic properties of the system. A insulator-semimetal transition is induced with external magnetic field.     

Analytical result of the effect of spin scattering and impurity-assistance on magnetoresistance in doped magnetic tunneling junctions

An extended tunneling Hamiltonian method is proposed to study the temperature-dependent tunneling magnetoresistance (TMR) in doped magnetic tunnel junctions. It is found that for nonmagnetic dopants (Si), impurity-assisted tunneling is mainly elastic, giving rise to a weak spin polarization, thereby reduces the overall TMR, while for magnetic ions (Ni), the collective excitation of local spins in δ-doped magnetic layer contributes to the severe drop of TMR and the behavior of the variation of TMR with temperature different from that for Si-doping. The theoretical results can reproduce the main characteristic features of experiments. Received 13 January 2002 / Received in final form 30 November 2002 Published online 6 March 2003 RID="a" ID="a"e-mail: yctao12@163.com     

Microscopic evidence of spin state order and spin state phase separation in layered cobaltites RBaCo2O5.5 with R=Y, Tb, Dy, and Ho

We report muon-spin relaxation measurements on the magnetic structures of RBaCo2O(5.5) with R=Y, Tb, Dy, and Ho. Three different phases, one ferrimagnetic and two antiferromagnetic, are identified below 300 K. They consist of different ordered spin state arrangements of high-, intermediate-, and low-spin Co3+ of CoO6 octahedra. Phase separation into well separated regions with different spin state order is observed in the antiferromagnetic phases. The unusual strongly anisotropic magnetoresistance and its onset at the FM-AFM phase boundary is explained.