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Optoplasmonic methods capable of single protein detection so far rely onanalyte immobilization in order to facilitate detection [1-6]. These detectionschemes, even if they facilitate transient single-molecule detection [7,8] viaconsequent formation and cleavage of chemical bonds, typically exhibit timeresolutions on the order of milliseconds. The need for analyte immobilisationis a direct consequence of the minuscule dimensions of plasmonic near fieldstypically providing sub-attolitre-sized detection volumes which in turn demandsub-microsecond temporal resolution for the direct detection of proteins inmotion. Here we show that such temporal resolution can indeed be achieved. Wedemonstrate the observation of single proteins as small as Hemoglobin(molecular weight: 64 kDa) as they traverse plasmonic near fields of goldnanorods and interact with their surface, all while maintaining signal-to-noiseratios larger than 5 and an unprecedented temporal resolution well belowmicroseconds. This method enables the label-free observation of single-moleculedynamics on previously unaccessible timescales.

Transient Optoplasmonic Detection of Single Proteins with Sub-Microsecond Resolution