We report observations to detect the 327 MHz line of atomic deuterium
in the primarily molecular clouds towards Cas A and Sgr A, making appr
opriate choices of spectral and spatial resolution. Our best results f
or Cas A, based on 1253 hr of observing with the 85 foot (26 m) Hat Cr
eek telescope and 45 hr with the VLA, yield an upper limit for the fra
ction of deuterium in atomic form, D I, of 0.14. We present an approxi
mate analytical analysis of deuterium fractionation in translucent clo
uds, which shows that gas-phase ion-molecule reactions, assisted by du
st and HD line self-shielding, are efficient in converting deuterium t
o HD. We conclude that little atomic deuterium is present in the molec
ular clumps in the Cas A clouds and that much higher sensitivity obser
vations would be required to detect the 327 MHz line in molecular clou
ds. We have also attempted to detect the 72 GHz line of DCO+ toward Ca
s A. The observed upper limit to the DCO+/HCO+ ratio of approximately
0.03 is not much larger than our theoretical estimate, and the DCO+ li
ne should be detectable with existing instrumentation, unless the temp
erature of these clouds is much larger than usually assumed.