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An ultrasensitive analytical method for direct detection of single nanoparticles in complex environment is described. The method relies on the wide-field surface plasmon microscopy (SPM). The suppression of matrix effects is achieved by image analysis based on the template matching. First, characteristic SPM images of nanoparticles are collected in aqueous suspensions. Then the detection of nanoparticles in complex environment is performed using template matching. Quantification and characterization of nanoparticles size was demonstrated at subppb level (∼100 pg/mL) in such complex media as wines, fruit juices, or cosmetic formulation. Visualization of the nanoparticles is performed in real time. The method does not require any sample pretreatment. If the minimally acceptable adsorption rate is defined as one nanoparticle to the whole sensor surface per few seconds, the working range of the method is ∼10 to 10 nanoparticles per mL.

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It has recently been shown that surface plasmon microscopy (SPM) allows single nanoparticles (NPs) on sensor surfaces to be detected and analyzed. The authors have applied this technique to study the adsorption of single metallic and plastic NPs. Binding of gold NPs (40, 60 and 100 nm in size) and of 100 nm polystyrene NPs to gold surfaces modified by differently ω-functionalized alkyl thiols was studied first. Self-assembled monolayers (SAM) with varying terminal functions including amino, carboxy, oligo(ethylene glycol), methyl, or trimethylammonium groups were deposited on gold films to form surfaces possessing different charge and hydrophobicity. The affinity of NPs to these surfaces depends strongly on the type of coating. SAMs terminated with trimethylammonium groups and carboxy group display highly different affinity and therefore were preferred when creating patterned charged surfaces. Citrate-stabilized gold NPs and sulfate-terminated polystyrene NPs were used as negatively charged NPs, while branched polyethylenimine-coated silver NPs were used as positively charged NPs. It is shown that the charged patterned areas on the gold films are capable of selectively adsorbing oppositely charged NPs that can be detected and analyzed with an ~1 ng⋅mL−1 detection limit. Graphical abstractSelf-assembled monolayers of ω-functionalized alkyl thiols were deposited on a gold layer of a patterned sensor array. The charge-selective binding of single nanoparticles to such surfaces was registered by wide-field surface plasmon microscopy. Electronic supplementary materialThe online version of this article (doi:10.1007/s00604-016-1956-7) contains supplementary material, which is available to authorized users.

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