Abstract
Visualized sensing through fluorescence signals is a powerful method for chemical and physical detection. However, the utilization of fluorescent molecular probes still suffers from lack of precise signal self-calibration in practical use. Here we show that fluorescence and thermally activated delayed fluorescence can be simultaneously produced at the single-molecular level. The thermally activated delayed fluorescence serves as a sensing signal with its wavelength and lifetime both altered correlating to polarity, whereas the fluorescence always remains unchanged as an internal reference. Upon the establishment of a three-dimensional working curve upon the ratiometric wavelength and photoluminescence lifetime vs. polarity, disturbance factors during a relevant sensing process can be largely minimized by such a multiple self-calibration. This strategy was further applied into a precise detection of the microenvironmental polarity variation in complex phospholipid systems, towards providing new insights for convenient and accurate diagnosis of membrane lesions.
Highlights
Visualized sensing through fluorescence signals is a powerful method for chemical and physical detection
A dualemission characteristic can be employed for ratiometric sensing, namely one emission providing an internal reference and the other acting as a sensing signal, on the basis of the spectral and temporal features
thermally activated delayed fluorescence (TADF) has been observed from intramolecular charge transfer (ICT) systems with a thermally accessible gap between the singlet and triplet excited states, enabling efficient up-conversion via thermally assisted reverse intersystem crossing (RISC)[15,16]
Summary
Visualized sensing through fluorescence signals is a powerful method for chemical and physical detection. Upon the establishment of a threedimensional working curve upon the ratiometric wavelength and photoluminescence lifetime vs polarity, disturbance factors during a relevant sensing process can be largely minimized by such a multiple self-calibration This strategy was further applied into a precise detection of the microenvironmental polarity variation in complex phospholipid systems, towards providing new insights for convenient and accurate diagnosis of membrane lesions. The wavelength and lifetime of the TADF signal changed along with environmental polarity, whereas the FL one stays insensitive, making it possible to establish a 3-D calibration method with ratiometric wavelength and lifetime vs polarity This strategy can be further applied for a precise detection of the microenvironmental polarity variation in complex phospholipid systems both in vitro and in vivo
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