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

被引:128
|
作者
Biggs, Kevin B. [1 ]
Camden, Jon P. [1 ]
Anker, Jeffrey N. [1 ]
Van Duyne, Richard P. [1 ]
机构
[1] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA
来源
JOURNAL OF PHYSICAL CHEMISTRY A | 2009年 / 113卷 / 16期
基金
美国国家科学基金会;
关键词
ION MOBILITY SPECTROMETRY; SENSITIVITY; SCATTERING; STABILITY;
D O I
10.1021/jp8112649
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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 (t(acq)) of 1 s. The DLt for this kinetically controlled sensor is fundamentally determined by the low sticking probability of BT on AgFONs which is determined to be similar to 2 x 10(-5) at 356 K. The sticking probability increases with increasing temperature consistent with an adsorption activation barrier of similar to 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 t(acq) = 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.
引用
收藏
页码:4581 / 4586
页数:6
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