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We report design, synthesis, and evaluation of fluorescent flipper probes for single-molecule super-resolution imaging of membrane tension in living cells.听听Reversible switching from bright-state ketones to dark-state hydrates, hemiacetals, and hemithioacetals is demonstrated for twisted and planarized mechanophores in solution and membranes.听听Broadband femtosecond fluorescence up-conversion spectroscopy听evinces ultrafast chalcogen-bonding cascade switching in the excited state in solution.听听According to听fluorescence lifetime imaging microscopy,听the new flippers image membrane tension听in live cells听with record red shifts and photostability.听听Single-molecule localization microscopy听with the new tension probes resolves membranes well below the diffraction limit.
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