The grille spectrometer observed the setting and rising sun 18 times during the Spacelab 1 mission. In addition to solar absorption lines, many of which had not been observed before, atmospheric spectral absorptions due to carbon monoxide and carbon dioxide were observed at heights tangent to the thermosphere (greater than 85km) , and absorptions due to ozone, water, methane, and nitrous oxide were observed in the mesosphere (greater than 50km). The strongly coupled molecules NO-NO2 and HCl-HF were observed as pairs in the stratosphere. Methane is presented as an example of the instrumental operations because of the characteristic aspect of the Q branch of its v3 band.