The research described in this dissertation is the first evaluation and application of a new class of optical detectors, two-dimensional charge-coupled device (CCD), for low-light level chemiluminescence and other luminescence spectroscopies. This research conclusively demonstrates the superior qualitative and quantitative performance of spectrometric systems which employ these detectors. It is experimentally shown that a single detector element of a CCD has comparable or superior sensitivity to the most sensitive single channel detectors; photomultiplier tubes (PMT). The results from the application of the CCD detector system to molecular spectroscopies (fluorescence, chemiluminescence, fluorescence detection of high performance liquid chromatography (HPLC) effluents, and chemiluminescence detection of HPLC effluents) and atomic spectroscopies (spatially and spectrally resolved spark and direct current plasma are presented). The results of operating the CCD in specialized readout modes developed in this research termed charge dependent variable binning (CDVB), simultaneous variable binning (SVB), and continuous high speed spectral framing (CHSF) are described and applied. The CDVB and SVB techniques allow very sensitive quantitation of spectrally resolved and unresolved signals with very wide dynamic ranges without prior knowledge of the signal intensity. Finally, CHSF technique provides spectrally resolved temporal study of extended period luminescence emission with millisecond time resolution. The results of unique algorithms to restore the integrity of the image obtained with a two-dimensional CCD detector are described and applied. The algorithms implemented are for removing variations in detector sensitivity and responsivity and spectrometer efficiency, as well as providing digital image filtering.
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