Understanding fracture
mechanics of ultrathin polymeric films is
crucial for modern technologies, including semiconductor and coating
industries. However, up to now, the fracture behavior of sub-100 nm
polymeric thin films is rarely explored due to challenges in handling
samples and limited testing methods available. In this work, we report
a new testing methodology that can not only visualize the evolution
of the local stress distribution through wrinkling patterns and crack
propagation during the deformation of ultrathin films but also directly
measure their fracture energies. Using ultrathin polystyrene films
as a model system, we both experimentally and computationally investigate
the effect of the film thickness and molecular weight on their fracture
behavior, both of which show a ductile-to-brittle transition. Furthermore,
we demonstrate the broad applicability of this testing method in semicrystalline
semiconducting polymers. We anticipate our methodology described here
could provide new ways of studying the fracture behavior of ultrathin
films under confinement.