
Dynamics of Core Electron Excitation and Decay in Molecules. Monochromatic
synchrotron radiation is used to excite molecules in molecular beams in
the region of the K edge of carbon, nitrogen, oxygen, and fluorine and
the L edge of silicon, sulfur, phosphorous, and chlorine. The excitation
is selective since the tightly bound core electrons of specific atoms can
be excited to distinct final state configurations. Core-hole excited state
symmetries and the photoabsorption anisotropy are determined from the angular
distribution of dissociation fragments. Electron-energy spectroscopy measures
branching ratios to different Auger, resonance Auger, and autoionization
pathways. Time-of-flight mass spectroscopy identifies dissociation products,
and electron-multiple ion coincidence techniques allow the dissociation
channels to be related to the electronic decay channels. Coincidence maps
provide information about the kinematics of the dissociation, including
angle, momentum, and kinetic energy distributions. Visible and ultraviolet
luminescence reveals neutral fragments created in excited electronic states
and serves as a high resolution probe of the Auger final state. Vibrational
and rotational branching ratios thus obtained provide information about
bond-length dependent properties of core-electron resonances, interference
effects resulting from lifetime broadening of the vibrational levels of
core-hole excited states, interchannel coupling of ionization continua,
and the partitioning of angular momentum.
Synchrotron Radiation Induced Chemistry in Films and on Surfaces. This
research is directed at elucidating novel chemical processes induced by
synchrotron radiation in the condensed phase. Such knowledge may prove
useful in microfabrication technology, specifically in the development
of high resolution or high sensitivity resists, in the development of resist-free
processing, and in the utilization of mild processing conditions. The photochemistry
induced by synchrotron radiation in condensed films, cryogenic matrices,
and surface adsorbates is monitored by Fourier transform infrared spectroscopy,
high resolution electron energy loss spectroscopy, and mass spectroscopy.
Etching and deposition rates are measured by laser interferometry. The
nature of the reactions, the reaction rates, and the dependence on photon
energy are of interest. The initial emphasis is on soft x-ray induced processes
and on determining the degree to which the chemistry is correlated with
the atomic site of the core-hole and the excited-state configuration. Subsequent
efforts will include the vuv region and studies leading to an understanding
of the electron and energy transfer processes that produce photochemistry
in a region around the excitation site.
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