Magnetic, thermoelectric, and electronic properties of layered oxides and carbon materials


Magnetic, thermoelectric, and electronic properties of layered oxides and carbon materials

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Title: Magnetic, thermoelectric, and electronic properties of layered oxides and carbon materials
Author: Caudillo, Roman, 1977-
Abstract: The structure and physical properties of layered oxides and carbon materials were studied. Two layered carbon materials were studied: carbon nanotubes (CNTs) synthesized by electron irradiation from amorphous carbon in situ in a transmission electron microscope (TEM) and a carbon and silver nanocomposite consisting of graphitic carbon nanospheres encapsulating Ag nanoparticles. In the CNT experiments, the effect of electron irradiation in the TEM is shown to alter drastically their structure and properties, even being able to transform amorphous carbon into a CNT. This suggests a possible alternative synthesis technique for the production of CNTs, in addition to providing a method for tailoring their properties. The structure and magnetic properties of the carbon and silver nanocomposite was characterized with x-ray diffraction, scanning and transmission electron microscopy techniques, and magnetic susceptibility measurements with a superconducting quantum interference device (SQUID) magnetometer. While the sp² bonding gives a grapheme sheet its mechanical properties, the p[subscript pi] electrons are responsible for its electronic and magnetic properties. In a flat graphene sheet the p[subscript pi] electrons are itinerant, but in a narrow p[subscript pi] band. The introduction of curvature to the graphene sheets that encapsulate the Ag nanoparticles is demonstrated to narrow the p[subscript pi] band sufficiently to result in "ferromagnetic" behavior. A model that is able to explain spin localization and ferrimagnetic spin-spin interactions in graphitic materials with positive curvature is presented. Layered oxides from the family of the P2 Na[subscript x]CoO₂ structure were synthesized and their properties studied. Na[subscript x]CoO₂ has a rich phase diagram ranging form a promising Na-rich thermoelectric composition to the hydrated Na-poor composition Na[subscript 0.33]CoO₂· 1.3H₂O that is superconductive. Intermediate to these two Na compositions exists an insulating phase with x [approximately equal to] 0.5 that presents a variety of interesting structural, magnetic, thermoelectric, and electronic behavior. Investigations of Na[subscript x]CoO₂ that probe the role of H₂O in the superconductive Na[subscript 0.33]CoO₂· 1.3H₂O are presented and conclude that H₂O plays a more active role than a passive lattice spacer. The relationship between Na ordering and an interesting magnetic behavior observed with [chi](T) measurements of annealed NaxCoO₂ and Sr[subscript x/2]CoO₂ samples is determined and found to correspond to a (2a x 2a) superstructure. The properties of NaxCoO₂ (x [approximately equal to] 0.5) are reviewed and thermoelectric S(T) measurements are made in order to develop a model that is able to explain the salient features of the NaxCoO₂ (x [approximately equal to] 0.5) phase.
Department: Materials Science and Engineering
Subject: Carbon Metallic oxides Nanoparticles
Date: 2007

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