Polymer–nanoparticle
(NP) hybrid nanocomposites act as essential
elements for ultraflexible memory devices due to their processability,
flexibility, and chemical resistance. However, a key limitation to
their potential is associated with their mechanical reliability with
the variation of temperature, which is still poorly understood. Herein,
we systematically investigated the temperature-dependent fatigue failure
of the Al/poly(9,9-dioctylfluorene-alt-benzothiadiazole)–ZnO/Al/PET
device, in which an 80% reduction in the fatigue lifetime of the device
was observed as the temperature decreased from 40 to −40 °C.
The finite element analysis results and theoretical calculations indicated
that polymer/NP interfaces play different roles in crack propagations
at different temperatures. At relatively high temperature, the elastic
mismatch at the polymer/NP interface allows it to alleviate the crack
propagation encountered with repetitive mechanical stress. However,
this behavior is suppressed by the significant decrease of the polymer
critical strain induced by the segmental motion in the polymer backbone
at low temperature. In this case, large stiffness mismatch at the
polymer/NP interface accelerates the crack propagation, which will
inhibit electron transfer and eventually lead to device breakdown.
This study may pave the way for future realization of ultraflexible
hybrid memory devices utilized in harsh environments.