Reversible gating of smart plasmonic molecular traps using thermoresponsive polymers for single-molecule detection

Yuanhui Zheng (), Alexander H. Soeriyadi, Lorenzo Rosa, Soon Hock Ng, Udo Bach and J. Justin Gooding ()
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Yuanhui Zheng: School of Chemistry, The University of New South Wales
Alexander H. Soeriyadi: School of Chemistry, The University of New South Wales
Lorenzo Rosa: Centre for Micro-Photonics (H34), Swinburne University of Technology
Soon Hock Ng: Monash University
Udo Bach: Monash University
J. Justin Gooding: School of Chemistry, The University of New South Wales

Nature Communications, 2015, vol. 6, issue 1, 1-8

Abstract: Abstract Single-molecule surface-enhanced Raman spectroscopy (SERS) has attracted increasing interest for chemical and biochemical sensing. Many conventional substrates have a broad distribution of SERS enhancements, which compromise reproducibility and result in slow response times for single-molecule detection. Here we report a smart plasmonic sensor that can reversibly trap a single molecule at hotspots for rapid single-molecule detection. The sensor was fabricated through electrostatic self-assembly of gold nanoparticles onto a gold/silica-coated silicon substrate, producing a high yield of uniformly distributed hotspots on the surface. The hotspots were isolated with a monolayer of a thermoresponsive polymer (poly(N-isopropylacrylamide)), which act as gates for molecular trapping at the hotspots. The sensor shows not only a good SERS reproducibility but also a capability to repetitively trap and release molecules for single-molecular sensing. The single-molecule sensitivity is experimentally verified using SERS spectral blinking and bianalyte methods.

Date: 2015
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DOI: 10.1038/ncomms9797

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