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Understanding the transmission of nanoscale forces in the pico-to-nanonewtonrange is important in polymer physics. While physical approaches havelimitations in analyzing the local force distribution in condensedenvironments, chemical analysis using force probes is promising. However, thereare stringent requirements for probing the local forces generated beforestructural damage. The magnitude of those forces corresponds to the range belowcovalent bond scission (from 200 pN to several nN) and above thermalfluctuation (several pN). Here, we report a conformationally flexibledual-fluorescence force probe with a theoretically estimated threshold ofapproximately 100 pN. This probe enables ratiometric analysis of thedistribution of local forces in a stretched polymer chain network. Withoutchanging the intrinsic properties of the polymer, the force distribution wasreversibly monitored in real time. Chemical control of the probe locationdemonstrated that the local stress concentration is twice as biased atcrosslinkers than at main chains, particularly in a strain-hardening region.Due to the high sensitivity, the percentage of stressed force probes wasestimated to be more than 1000 times higher than the activation rate of aconventional mechanophore.

Bridging Pico-to-Nanonewtons with a Ratiometric Force Probe for Monitoring Nanoscale Polymer Physics Before Damage