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Abstract Most elastomers undergo strain‐induced crystallization (SIC) under tension; as individual chains are held rigidly in a fixed position by an applied strain, their alignment along the strain field results in a shift from strain‐hardening (SH) to SIC. A similar degree of stretching is associated with the tension necessary to accelerate mechanically coupled, covalent chemical responses of mechanophores in overstretched chains, raising the possibility of an interplay between the macroscopic response of SIC and the molecular response of mechanophore activation. Here, thiol‐yne‐derived stereoelastomers doped covalently with a dipropiolate‐derivatized spiropyran (SP) mechanophore (0.25–0.38 mol%) are reported. The material properties of SP‐containing films are consistent with undoped controls, indicating that the SP is a reporter of the mechanical state of the polymer. Uniaxial tensile tests reveal correlations between mechanochromism and SIC, which are strain‐rate‐dependent. When mechanochromic films are stretched slowly to the point of mechanophore activation, the covalently tethered mechanophore remains trapped in a force‐activated state, even after the applied stress is removed. Mechanophore reversion kinetics correlate with the applied strain rate, resulting in highly tunable decoloration rates. Because these polymers are not covalently crosslinked, they are recyclable by melt‐pressing into new films, increasing their potential range of strain‐sensing, morphology‐sensing, and shape‐memory applications. 

Abstract Room‐temperature solution‐processed flexible photodetectors with spectral response from 300 to 2600 nm are reported. Solution‐processed polymeric thin film with transparency ranging from 300 to 7000 nm and superior electrical conductivity as the transparent electrode is reported. Solution‐processed flexible broadband photodetectors with a “vertical” device structure incorporating a perovskite/PbSe quantum dot bilayer thin film based on the above solution‐processed transparent polymeric electrode are demonstrated. The utilization of perovskite/PbSe quantum dot bilayer thin film as the photoactive layer extends spectral response to infrared region and boosts photocurrent densities in both visible and infrared regions through the trap‐assisted photomultiplication effect. Operated at room temperature and under an external bias of ‐1 V, the solution‐processed flexible photodetectors exhibit over 230 mA W^‐1responsivity, over 1011 cm Hz1/2/W photodetectivity from 300 to 2600 nm and ≈70 dB linear dynamic ranges. It is also found that the solution‐processed flexible broadband photodetectors exhibit fast response time and excellent flexibility. All these results demonstrate that this work develop a facile approach to realize room‐temperature operated ultrasensitive solution‐processed flexible broadband photodetectors with “vertical” device structure through solution‐processed transparent polymeric electrode.