The frequency-dispersed birefringence and dichroism of an
electronically nonresonant liquid excited and probed
by ultrafast pulses in an optically heterodyned detected configuration
is reported. The nominally putative
dichroic response of a transparent sample is shown to result from π
out-of-phase contributions of Stokes and
anti-Stokes third-order polarization components on, respectively, the
red and blue sides of the probe pulse
spectrum and are derived from CSRS and CARS type resonances. The
strong corresponding nondispersed
birefringent response, in contrast, results from the in-phase
combination of these Stokes and anti-Stokes
polarization components. Thus, by observing the dispersed probe
pulse to the red or blue of the central
carrier frequency, the various density matrix components, or pathways
in time evolution history, contributing
to either a dichroic or birefringent measurement may be more
selectively viewed. The contribution of a
particular nuclear response is enhanced when the observed frequency
within the probe pulse spectrum is
tuned to be either one quantum to the red or blue of the carrier
frequency. This frequency-filtering technique
can be used to enhance weak features in the total response, allow the
determination of isotropic and anisotropic
contributions to a nuclear response, and help probe the homogeneous and
inhomogeneous character of the
low-frequency Raman active density of states commonly observed in these
two-pulse responses of nonresonant
liquids. These effects are illustrated by the OHD birefringence
and dichroism of CHCl3.
In this paper, we report on the synthesis and characterization of cobalt aggregates electrochemically incorporated on composite polypyrrole films. XAS (X-ray absorption spectroscopy) was used to probe the atomic local order in these composites and to furnish new insights into the metal/polymer interaction. A complete understanding of the incorporation process and its evolution was achieved by in situ XAS measurements at different stages of the electrochemical process. These results indicate that the reaction starts with the Co 2+ entrapped in the polymeric matrix as a complex [-[(C 4 H 2 N) 3 CH 3 (CH 2 ) 11 OSO 3 -] 6 Co 2+ ]. The reduction of this complex leads to the synthesis of Co aggregates in the film. Measurements at the O and N K edges evidence that the main interaction between Co aggregates and the polymer is verified via Co-N bonds, the N originating from the polypyrrole (PPy) amine group. The pH effect on the metal/polymer interaction is discussed. Scanning electron microscopy (SEM) measurements show the formation of dendritic-like cobalt aggregates on the film surface. The magnetic response obtained by in situ alternating gradient field magnetometry (AGFM) allows prediction of the possibility of obtaining a magnetic polymer with superparamagnetic particles with sizes below 10 nm. Our results are the first steps toward the development of an advanced material with exciting potential for future recording media application.
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