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We investigated the individual properties of various polyion-coated bubbleswith a mean diameter ranging from 300 to 500 nm. Dark field microscopy allowsone to track the individual particles of the submicron bubbles (SBs)encapsulated by the layer-by-layer (LbL) deposition of cationic and anionicpolyelectrolytes (PEs). Our focus is on the two-step charge reversals of PE-SBcomplexes: the first is a reversal from negatively charged bare SBs with no PEsadded to positive SBs encapsulated by polycations (monolayer deposition), andthe second is overcharging into negatively charged PE-SB complexes due to thesubsequent addition of polyanions (double-layer deposition). The details ofthese phenomena have been clarified through the analysis of a number oftrajectories of various PE-SB complexes that experience either Brownian motionor electrophoresis. The contrasted results obtained from the analysis were asfollows: an amount in excess of the stoichiometric ratio of the cationicpolymers was required for the first charge-reversal, whereas the stoichiometricaddition of the polyanions lead to the electrical neutralization of the PE-SBcomplex particles. The recovery of the stoichiometry in the double-layerdeposition paves the way for fabricating multi-layered SBs encapsulated solelywith anionic and cationic PEs, which provides a simple protocol to create smartagents for either drug delivery or ultrasound contrast imaging.

Microscopic Characterization of Individual Submicron Bubbles during the Layer-by-Layer Deposition: Towards Creating Smart Agents