Ratiometric Flapping Force Probe That Works in Polymer Gels

09 December 2021, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

A ratiometric flapping force probe that can evaluate the nanoscale stress concentration in the polymer chain network of common organogels has been developed. Stress-dependent dual-fluorescence properties of the chemically doped flapping force probe has been demonstrated even when the probe is solvated in the wet materials (Figure 1). The fluorescence ratiometric analysis is robust against the local concentration change induced by the macroscopic polymer deformation. While the force-responsive FRET dyads, widely used in mechanobiology, are sensitive to the distance and orientation of the two chromophores, the flapping fluorophore works as a single-component flexible force probe regardless of the FRET efficiency. Realtime and reversible spectral response to the mechanical stress is observed with a low threshold on the order of sub-MPa compression due to its conformational flexibility. The previously reported flapping probe only shows a negligible response in the solvated environments because the undesired spontaneous planarization occurs in the S1 excited state, even without mechanical force. The excited-state engineering by changing the flapping wings from the anthraceneimide units to the pyreneimide units endows this molecule with the force probe function in the wet conditions. The structurally modified force probe also has an advantage in terms of a wide dynamic range of the fluorescence response in solvent-free elastomers, which enabled the ratiometric fluorescence imaging of the molecular-level stress concentration during the crack growth in a stretched polyurethane film. The percentage of the stressed force probes has been experimentally estimated to be approximately 30–40% before the fracture of the elastomers. The flapping force probe is useful for elucidating the toughening mechanism of recently focused unique topological gels and elastomers at molecular level.

Keywords

force probe
mechanochemistry
dual fluorescence
polymer gels
flapping molecules

Supplementary materials

Title
Description
Actions
Title
Supporting Movie 1
Description
Reversible fluorescence response of the SPU1 film.
Actions
Title
Supporting Movie 2
Description
Ratiometric fluorescence imaging of the notched SPU1 film in the tensile test.
Actions
Title
Supporting Movie 3
Description
Compression process of the cylindrical specimen of Gel1.
Actions
Title
Supporting Movie 4
Description
Stress mapping of the compressed organogels by ratiometric fluorescence imaging.
Actions

Comments

Comments are not moderated before they are posted, but they can be removed by the site moderators if they are found to be in contravention of our Commenting Policy [opens in a new tab] - please read this policy before you post. Comments should be used for scholarly discussion of the content in question. You can find more information about how to use the commenting feature here [opens in a new tab] .
This site is protected by reCAPTCHA and the Google Privacy Policy [opens in a new tab] and Terms of Service [opens in a new tab] apply.