Gelation of gelatin under various conditions has been followed by atom
ic force microscopy (AFM) with the objective of understanding more ful
ly the structure formed during the gelation process. AFM images were o
btained of the structures formed from both the bulk sol and in surface
films during the onset of gelation. While gelation occurred in the bu
lk sol, the extent of helix formation was monitored by measurements of
optical rotation, and the molecular aggregation was imaged by AFM. In
terfacial gelatin films formed at the air-water interface were also st
udied Measurements of surface tension and surface rheology were made p
eriodically and Langmuir-Blodget films were drawn from the interface t
o allow AFM imaging of the structure of the interfacial layer as a fun
ction of time. Structural studies reveal that at low levels of helical
content the gelatin molecules assemble into aggregates containing sho
rt segments of dimensions comparable to those expected for gelatin tri
ple helices. With time larger fibrous structures appear whose dimensio
ns suggest that they are bundles of triple helices. As gelation procee
ds, the number density of fibers increases at the expense of the small
er aggregates, eventually assembling into a fibrous network. The gel s
tructure appears to be sensitive to the thermal history, and this is p
articularly important in determining the structure and properties of t
he interfacial films. (C) 1998 John Wiley & Sons, Inc.