A vibrational analysis has been carried out to analyze the chain conformati
on of poly(lactic acid) in the crystalline state. In conjunction with a nor
mal-coordinate analysis, the Raman spectrum has yielded data regarding conf
ormational distributions. Raman spectra of different helices were simulated
using previously published structures, force constants, and intensity para
meters. Some of the chain conformations predicted are inconsistent with the
data. Only one of the four 3(1) helical structures predicted by conformati
onal analysis agrees well with experiment. This analysis provides a new und
erstanding regarding the relative probability of a 10(3) or 3(1) helix for
poly(lactic acid).