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In situ electrochemical regeneration of nanogap hotspots for continuously reusable ultrathin SERS sensors.


ABSTRACT: Surface-enhanced Raman spectroscopy (SERS) harnesses the confinement of light into metallic nanoscale hotspots to achieve highly sensitive label-free molecular detection that can be applied for a broad range of sensing applications. However, challenges related to irreversible analyte binding, substrate reproducibility, fouling, and degradation hinder its widespread adoption. Here we show how in-situ electrochemical regeneration can rapidly and precisely reform the nanogap hotspots to enable the continuous reuse of gold nanoparticle monolayers for SERS. Applying an oxidising potential of +1.5 V (vs Ag/AgCl) for 10 s strips a broad range of adsorbates from the nanogaps and forms a metastable oxide layer of few-monolayer thickness. Subsequent application of a reducing potential of -0.80 V for 5 s in the presence of a nanogap-stabilising molecular scaffold, cucurbit[5]uril, reproducibly regenerates the optimal plasmonic properties with SERS enhancement factors ≈106. The regeneration of the nanogap hotspots allows these SERS substrates to be reused over multiple cycles, demonstrating ≈5% relative standard deviation over at least 30 cycles of analyte detection and regeneration. Such continuous and reliable SERS-based flow analysis accesses diverse applications from environmental monitoring to medical diagnostics.

SUBMITTER: Sibug-Torres SM 

PROVIDER: S-EPMC10917746 | biostudies-literature | 2024 Mar

REPOSITORIES: biostudies-literature

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In situ electrochemical regeneration of nanogap hotspots for continuously reusable ultrathin SERS sensors.

Sibug-Torres Sarah May SM   Grys David-Benjamin DB   Kang Gyeongwon G   Niihori Marika M   Wyatt Elle E   Spiesshofer Nicolas N   Ruane Ashleigh A   de Nijs Bart B   Baumberg Jeremy J JJ  

Nature communications 20240306 1


Surface-enhanced Raman spectroscopy (SERS) harnesses the confinement of light into metallic nanoscale hotspots to achieve highly sensitive label-free molecular detection that can be applied for a broad range of sensing applications. However, challenges related to irreversible analyte binding, substrate reproducibility, fouling, and degradation hinder its widespread adoption. Here we show how in-situ electrochemical regeneration can rapidly and precisely reform the nanogap hotspots to enable the  ...[more]

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