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The fracture of polymer materials is a multiscale process starting with the scission of a single molecular bond advancing to a site of failure within the bulk. Quantifying the bonds broken during this process remains a big challenge yet would help to understand the distribution and dissipation of macroscopic mechanical energy. We here show the design and synthesis of fluorogenic molecular optical force probes (mechanofluorophores) covering the entire visible spectrum in both absorption and emission. Their dual fluorescent character allows to track non‐broken and broken bonds in dissolved and bulk polymers by fluorescence spectroscopy and microscopy. Importantly, we develop an approach to determine the absolute number and relative fraction of intact and cleaved bonds with high local resolution. We anticipate that our mechanofluorophores in combination with our quantification methodology will allow to quantitatively describe fracture processes in materials ranging from soft hydrogels to high‐performance polymers., A new platform of dual fluorescent mechanofluorophores that display covalent bond scission during material breakage by changing their optical properties was synthesized. The absorption and emission characteristics were tuned to cover the entire visible spectrum. Using photon quantitative confocal fluorescence microscopy, these new mechanofluorophores enabled the quantification of bond scission events with μm resolution.

The 3D structure and the local environment of stimuli-responsive microgels were investigated with the superresolution fluorescence microscopy method PAINT using Nile Red as solvatochromic dye., Polymer nanostructures have enormous potential for various applications in materials and life sciences. In order to exploit and understand their full capabilities, a detailed analysis of their structures and the environmental conditions in them is essential on the nanoscopic scale. With a super-resolution fluorescence microscopy technique known as PAINT (Points Accumulation for Imaging in Nanoscale Topography), we imaged colloidal hydrogel networks, so-called microgels, having a hydrodynamic radius smaller than the diffraction limit, gaining unprecedented insight into their full 3D structure which is not accessible in this much detail with any other experimental method. In addition to imaging of the microgel structure, the use of Nile Red as the solvatochromic fluorophore allowed us to resolve the polarity conditions within the investigated microgels, thus providing nanoscopic information on the x,y,z-position of labels including their polarity without the need of covalent labelling. With this imaging approach, we give a detailed insight into adapting structural and polarity properties of temperature-responsive microgels when changing the temperature beyond the volume phase transition.