Molecular deformation processes of regenerated cellulose fibers are investi
gated using Raman spectroscopy. These fibers have well-defined Raman spectr
a, and the main Raman bands in tho region of 895 to 1170 cm(-1) shift to lo
wer wavenumbers upon application of tensile strain and stress. The peak pos
itions of the Raman bands at 895 and 1095 cm(-1) show an approximately line
ar relationship with strain and stress. For fibers with lower moduli and mo
re nonlinearity in their stress-strain curves, there is poorer correlation
with strain and stress, consistent with mechanical data and structural char
acteristics. Also, the strain sensitivity of the Raman band strain shift (i
n cm(-1)/%) increases with the Young's modulus of regenerated cellulose fib
ers, and there is a universal stress band shift of about -4 cm(-1)/GPa for
both bands, consistent with a modified series model of deformation. Deviati
ons from this model for lower fiber moduli are discussed with evidence to s
uggest that chain slippage and re-orientation behavior dominate.