Isotopic (delta(17)O and delta(18)O) measurements of stratospheric and
mesospheric carbon dioxide (CO2) and oxygen (O-2), along with trace s
pecies concentrations (N2O, CO, and CO2), were made in samples collect
ed from a rocket-borne cryogenic whole air sampler. A large mass-indep
endent isotopic anomaly was observed in CO2, which may in part derive
from photochemical coupling to ozone (O-3). The data also require an a
dditional isotopic fractionation process, which is presently unidentif
ied. Mesospheric O-2 isotope ratios differed from those in the troposp
here and stratosphere. The cause of this isotopic variation in O-2 is
presently unknown. The inability to account for these observations rep
resents a fundamental gap in the understanding of the O-2 chemistry in
the stratosphere and mesosphere.