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The improved initialization inversion (3I) algorithms convert TIROS-N Operational Vertical Sounder observations from the National Oceanic and Atmospheric Administration (NOAA) polar-orbiting environmental satellites into atmospheric temperature and water vapor profiles, together with cloud and surface properties. Their relatively good spectral resolution and coverage make IR sounders a very useful tool for the determination of cloud properties both day and night. The iterative process of detailed comparisons between cloud parameters obtained from this global dataset, which is available in the framework of the NOAA-National Aeronautics and Space Administration Pathfinder Program, with time-space-collocated observations of clouds from the recently reprocessed international Satellite Cloud Climatology Project (ISCCP) dataset has led to an improved 3I cloud analysis scheme based on a weighted-chi(2) method described in the second article of this series. This process also provides a first evaluation of the ISCCP reanalysis. The new 3I cloud scheme obtains cloud properties very similar to those from ISCCP for homogeneous cloud scenes. Improvement is especially notable in the stratocumulus regimes where the new 3I scheme detects much more of the low-level cloudiness. Remaining discrepancies in cloud classification can now be explained by differences in cloud detection sensitivity, differences in temperature profiles used, and inhomogeneous or partly cloudy fields. Cirrus cloud identification during the daytime in the recent ISCCP dataset is improved relative to the first version of ISCCP, but is still an underestimate. At night only multispectral IR analyses like 3I can provide cirrus information. The reprocessed ISCCP dataset also shows considerable improvement in cloud cover at higher latitudes. Differences in 3I and ISCCP summertime cloud cover over deserts may be caused by different sensitivities to dust storms.