Microstructure, chemical composition, and dielectric response of CaCu3Ti4O12 ceramics doped with F, Al, and Mg ions.

Ceramics with nominal chemical composition CaCu3Ti4O12 (CCTO), CaCu3Ti3.96Al0.04O11.96F0.04 (CCTOAF), and Ca0.98Mg0.08Cu2.94Ti3.96Al0.04O11.96F0.04 (CCTOMAF) were prepared by the solid-state reactions technique. Using SEM, EDX, XPS, EPR, NMR, and complex impedance spectroscopy, the microstructure, elements distribution, chemical composition of grains and grain boundaries, and the dielectric response of ceramics were investigated. In the ССТО, CCTOAF, and CCTOMAF series, the average grain size increases, the degree of copper segregation at the grain boundaries is inversely related to grain size, and the dielectric loss decreases from 0.071 to 0.047 and 0.030, respectively, while dielectric permittivity ε' at 1 kHz is 5.6 × 104, 7.1 × 104, and 4.3 × 104, respectively. Additives of Al, Mg, F and milled particles (ZrO2, Al2O3, and SiO2) can either partially introduce into the perovskite structure or form low-melting eutectics at the grain boundaries, causing abnormal grain growth. The presence of copper ions in various oxidation states, as well as evidence of exchange spin interactions between them, was confirmed in all samples.

Critical behavior of ensembles of superparamagnetic nanoparticles with dispersions of magnetic parameters.

Different processes governing magnetic properties of an ensemble of magnetic nanoparticles in the temperature region close to a transition from superparamagnetic to paramagnetic state are analyzed and the ways to separate them are suggested. Enhanced role of paraprocess in magnetization behavior near Curie temperature is stressed. A procedure to isolate paraprocess contribution and adequately determine spontaneous magnetization of the ensemble of superparamagnetic nanoparticles is proposed. Critical behavior of the spontaneous magnetization is experimentally determined for the ensemble of nanoparticles of lanthanum-strontium manganites, which are considered as promising materials for self-controlled magnetic nanohyperthermia. Effect of dispersion of magnetic parameters on effective magnetic characteristics of nanoparticles and their critical behavior is discussed. Theoretical background for the use of the 'effective Curie temperature for the ensemble of nanoparticles' concept is proposed for ensembles of particles with dispersion of their Curie temperature. Based on the results obtained, various strategies to develop novel biomedical applications, in particular those suitable for noninvasive temperature monitoring, are discussed.

Interplay between superparamagnetic and blocked behavior in an ensemble of lanthanum-strontium manganite nanoparticles.

Magnetic nanoparticles constitute promising tools for addressing medical and health-related issues based on the possibility to obtain various kinds of responses triggered by safe remote stimuli. However, such richness can be detrimental if different performances are not adequately differentiated and controlled. The aim of this work is to understand and systemize different kinds of magnetic-field-induced response for an ensemble of lanthanum-strontium manganite nanoparticles, which are considered as promising materials for self-controlled magnetic hyperthermia. A complex set of static and dynamic magnetic measurements accompanied by a numerical simulation of DC and AC magnetic behavior has been carried out. It is shown that to achieve adequate results, the dispersion of particle sizes and/or magnetic parameters should necessarily be taken into account. A quantitative description of the magnetic behavior of the ensemble should comprise two groups of nanoparticles differentiated according to the regime of their magnetization reversal: one group, which demonstrates non-hysteretic behavior similar to a superparamagnet and another one, which shows magnetic hysteresis characteristic of blocked particles. The fraction of nanoparticles in each group depends not only on the nanoparticles' parameters (in particular, their size), but also on the parameters of the external AC magnetic field (amplitude and frequency) used for remagnetization. The main outcome of this work is the development of a procedure which allows one to separately analyze contributions from different groups of nanoparticles and find the regularities of the redistribution of nanoparticles between these groups on changing the parameters of the external AC magnetic field. The results show the directions to enhance the heating efficiency of ensembles of magnetic nanoparticles and pave the way for further optimization of their characteristics and the parameters of the external field.

Mechanisms of AC losses in magnetic fluids based on substituted manganites.

The ability to controllably tune the heating efficiency of magnetic nanoparticles in an AC magnetic field is highly desirable for their application as mediators of magnetic hyperthermia. Traditional approaches to understand and govern the behavior of hyperthermia mediators include a combination of quasistatic and high-frequency (∼100 kHz) magnetic measurements with subsequent simulation of underlying processes. In this paper, we draw attention to the frequently overlooked fact that for an ensemble of magnetic nanoparticles, there is no straightforward complementarity between the dynamic characteristics obtained under different experimental conditions, as well as between corresponding underlying processes. This paper analyzes mechanisms of AC losses in a fluid based on magnetic nanoparticles, with special emphasis on the domains of their validity, and shows that the mechanisms may become qualitatively different as experimental conditions change from magnetostatic to high-frequency ones. Further, the work highlights new important features which can result from the employment of the refined approaches to interpret experimental results obtained on magnetic fluids based on La1-xSrxMnO3 (x = 0.22) nanoparticles. The gained knowledge provides necessary guidelines for tailoring the properties of magnetic nanoparticles to the needs of self-controlled magnetic hyperthermia.

Mössbauer study and magnetic properties of M-type barium hexaferrite doped with Co + Ti and Bi + Ti ions.

Using X-ray powder diffractions, Mössbauer spectroscopy, and magnetic measurements, the effect of complex dopants (Co2+ + Ti4+) and (Bi3+ + Ti4+) on the fine structure and magnetic properties of M-type barium hexaferrite prepared by hydroxide and carbonate precipitations has been studied. The distribution of cations over five nonequivalent positions of barium hexaferrite with magnetoplumbite structure is discussed. It has been shown that doped barium hexaferrite can be used for high-coercitivity data storage media.

Influence of vacancy ordering on the percolative behavior of (Li(1)(-x)Na(x))(3y)La(2/3-y)TiO(3) perovskites.

Influence of the vacancy concentration on the Li conductivity of the (Li(1-x)Na(x))(0.2)La(0.6)TiO(3) and (Li(1-x)Na(x)(0.5)La(0.5)TiO(3) perovskite series, with 0 < or = x < 1, has been investigated by neutron diffraction (ND), impedance spectroscopy (IS), nuclear magnetic resonance (NMR), and Monte Carlo simulations. In both series, Li(+) ions occupy unit cell faces, but Na(+) ions are located at A sites of the perovskite. From this fact, the amount of vacant A sites that participate in Li conductivity is given by the expression n(v) = [Li] + square, where square is the nominal vacancy concentration. Substitution of Li by Na decreases the amount of vacancies, reducing drastically the Li conductivity when n(v) approaches the percolation threshold of the perovskite conduction network. In disordered (Li(1-x)Na(x))(0.5)La(0.5)TiO(3) perovskites, the percolation threshold is 0.31; however, in ordered (Li(1-x)Na(x))(0.2)La(0.6)TiO(3) perovskites, this parameter changes to 0.26. Near the percolation threshold, the amount of mobile Li species deduced by (7)Li NMR spectroscopy is lower than that derived from structural formulas but higher than deduced from dc conductivity measurements. Conductivity values have been explained by Monte Carlo simulations, which assume a random walk for Li ions in the conduction network of the perovskite. In these simulations, distribution of vacancies conforms to structural models deduced from ND experiments.