Polymer gels have
recently attracted attention for their application
in flexible devices, where mechanically robust gels are required.
While there are many strategies to produce tough gels by suppressing
nanoscale stress concentration on specific polymer chains, it is still
challenging to directly verify the toughening mechanism at the molecular
level. To solve this problem, the use of the flapping molecular force
probe (FLAP) is promising because it can evaluate the nanoscale forces
transmitted in the polymer chain network by ratiometric analysis of
a stress-dependent dual fluorescence. A flexible conformational change
of FLAP enables real-time and reversible responses to the nanoscale
forces at the low force threshold, which is suitable for quantifying
the percentage of the stressed polymer chains before structural damage.
However, the previously reported FLAP only showed a negligible response
in solvated environments because undesirable spontaneous planarization
occurs in the excited state, even without mechanical force. Here,
we have developed a new ratiometric force probe that functions in
common organogels. Replacement of the anthraceneimide units in the
flapping wings with pyreneimide units largely suppresses the excited-state
planarization, leading to the force probe function under wet conditions.
The FLAP-doped polyurethane organogel reversibly shows a dual-fluorescence
response under sub-MPa compression. Moreover, the structurally modified
FLAP is also advantageous in the wide dynamic range of its fluorescence
response in solvent-free elastomers, enabling clearer ratiometric
fluorescence imaging of the molecular-level stress concentration during
crack growth in a stretched polyurethane film.