The phase content and crystallinity of initially amorphous amylose-water mi
xtures (70/30 W/W) have been changed by slow cycles of dissolution and recr
ystallization from T-max with 50 degrees C < T-max < 120 degrees C. Analysi
s of the treatment-induced changes is made by X-ray diffraction, FTIR, fast
T-ramp DSC and slow calorimetry. Our interest was to follow the relaxation
of the network phase and its consequence on the growth of crystallinity. T
he DSC technique, which gives the temperature of disappearance of long-rang
e order, is unable to quantitatively follow the growth of crystallinity ach
ieved by treating the samples. In highly interactive polymer-solvent system
s, order is unmeltable in a fast T-ramp due to strain developed during the
ramp. In a 6 K/h T-ramp, the order becomes meltable and grows from 21 J/g t
o 147 J/g when T-max increases. The other conclusion is that strain-melting
and the network phase, characterized first in polyolefins has a more promi
nent role in the characterization of H-bonded polysaccharide-water mixtures
. Correlation is achieved between the concentration of bands in the C-O str
etching region, the fraction of single and double helices, and the three en
dotherms found on the slow T-ramp dissolution traces. FTIR spectra show tha
t chains in the network cannot be disentangled by quenching but can be orga
nized during a slow cooling. The B and V crystalline modifications are obse
rved in the treated samples. Quenched treated amylose and enzyme-resistant
amylose seem to contain a comparable amount of double-helical/strainable fr
action. (C) 2000 John Wiley & Sons, Inc.