Surface-enhanced raman spectroscopy of benzenethiol adsorbed from the gas phase onto silver film over nanosphere surfaces: Determination of the sticking probability and detection limit time

Kevin B. Biggs, Jon P. Camden, Jeffrey N. Anker, Richard P.Van Duyne

Research output: Contribution to journalArticlepeer-review

118 Scopus citations

Abstract

A chemical warfare agent (CWA) gas detector based on surface-enhanced Raman spectroscopy (SERS) using robust nanostructured substrates and a portable Raman spectrometer is a promising alternative to existing modalities. A gas-dosing apparatus was constructed to simulate chemical gas exposure and provide a platform for quantitative analysis of SERS detection. As a first step toward characterizing SERS detection from the gas phase, benzenethiol (BT) has been chosen as the test analyte. SERS spectra were monitored during BT adsorption onto a silver film over a nanosphere (AgFON) substrate. The SERS detection limit time (DLt) for BT on a AgFON at 356 K is found to be 6 ppm-s (30 mg-s m-3) for a data acquisition time (tacq)of1s.The DLt for this kinetically controlled sensor is fundamentally determined by the low sticking probability of BT on AgFONs which is determined to be ∼2 x 10-5 at 356 K. The sticking probability increases with increasing temperature consistent with an adsorption activation barrier of ∼13 kJ mol-1. Although the DLts found in the present study for BT are in the low ppm-s, a theoretical model of SERS detection indicates DLts below 1 ppb s-1 for tacq= 1 s are, in fact, achievable using existing portable Raman instrumentation and AgFON surfaces. Achieving this goal requires the sticking probability be increased 3 orders of magnitude, illuminating the importance of appropriate surface functionalization.

Original languageEnglish (US)
Pages (from-to)4581-4586
Number of pages6
JournalJournal of Physical Chemistry A
Volume113
Issue number16
DOIs
StatePublished - Apr 23 2009

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

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