Self-assembly of Au nanocrystals into large-area 3-D ordered flexible superlattice nanostructures arrays for ultrasensitive trace multi-hazard detection.

Plasmonic nanoparticles that self-assemble into highly ordered superlattice nanostructures hold substantial promise for facilitating ultra-trace surface-enhanced Raman scattering (SERS) detection. Herein, we propose a boiling-point evaporation method to synthesize ordered monocrystal-like superlattice Au nanostructures (OML-Au NTs) with a polyhedral morphology. Combined with thermal nanoimprint technology, OML-Au NTs were directly transferred to impact-resistant polystyrene (IPS) flexible SERS substrates, the obtained flexible substrates (donated as OML-Au NTs/IPS) detection limit for R6G molecules as low as 10 ^-13 M. These results were confirmed by simulating the electromagnetic field distribution of ordered/unordered two-dimensional single-layer and three-dimensional aggregated gold nanostructures. The OML-Au NTs/IPS substrates were successfully used to detect and quantify three commonly-used agricultural pesticides, achieving detection limits as low as 10 ^-11 M and 10 ^-12 M, and in situ real-time detection limit reached 0.24 pg/cm ² for thiram on apple peels, which was 3 orders of magnitude lower than the current detection limit. In addition, the Raman intensity from multiple locations showed a relative standard deviation lower than 7 %, exhibiting the reliability necessary for practical applications. As a result, this research demonstrates a highly reproducible method to enable the development of plasmonic nanomaterials with flexible superstructures.
Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
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