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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.ÌýÌýReversible switching from bright-state ketones to dark-state hydrates, hemiacetals, and hemithioacetals is demonstrated for twisted and planarized mechanophores in solution and membranes.ÌýÌýBroadband femtosecond fluorescence up-conversion spectroscopyÌýevinces ultrafast chalcogen-bonding cascade switching in the excited state in solution.ÌýÌýAccording toÌýfluorescence lifetime imaging microscopy,Ìýthe new flippers image membrane tensionÌýin live cellsÌýwith record red shifts and photostability.ÌýÌýSingle-molecule localization microscopyÌýwith the new tension probes resolves membranes well below the diffraction limit.
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