Materials prepared by syndiotactic polypropylene of different stereoch
emistry (62 divided by 96% r pentads) undergo transitions in the cryst
al phase, which depend on the thermomechanical history. The interfaces
and the amorphous phase may be affected by the crystallite organizati
on and the stereoregularity of the material. MAS NMR techniques provid
ed a tool for characterizing the arrangement and the mobility of the p
olymer chains in the inter-crystallite region. Chemical shifts, line-w
idth and relaxation parameters were determined as a function of record
ing temperature and glass transition temperature of the material. The
same parameters were followed in the presence of a plasticizer. The di
fferent degree of intimacy of the phases was established by following
the diffusion of magnetization among the hydrogen atoms of the amorpho
us and the crystalline phase. Defective regions and boundary regions w
ere also identified and showed a large amount of conformations in the
trans arrangement; the relaxation times indicate the chains being rigi
d and intimately mixed with the crystalline phase.