The Mossbauer spectroscopy has been applied to high density polyacetyl
ene films doped with I-129. In addition to the well-known polyiodide a
nions, I3- and I5-, a new iodine species Ialpha has been found in the
present study. The new species Ialpha has been assigned to the iodine
atom covalently bound to the chain carbon. Although the iodine Ialpha
introduces sp3-carbon defects interrupting the alternation of single a
nd double bonds of the chain, the amount of Ialpha has been estimated
to be lower than a critical sp3-carbon concentration which is a theore
tically predicted value to break the highly conductive phase of iodine
-doped polyacetylene. From the angular dependent Mossbauer spectra obt
ained under the condition that the oriented direction of the polymer i
s parallel and perpendicular to the propagating direction of the incid
ent gamma-rays, it has been revealed that the molecular axes of I3- an
d I5- are aligned along the oriented direction of the polymer.