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Cited by 1,078

The DOI matches its Crossref record; 54 of the 54 references it cites were found in a registry or an index.

Chain Length Dependence and Sensing Capabilities of the Localized Surface Plasmon Resonance of Silver Nanoparticles Chemically Modified with Alkanethiol Self-Assembled Monolayers

Malinsky, Michelle Duval, Kelly, K. Lance, Schatz, George C., Van Duyne, Richard P.·2001·Journal of the American Chemical Society
DOI 10.1021/ja003312a
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Abstract

In this paper, we explore the optical properties of Ag nanoparticles chemically modified with alkanethiol self-assembled monolayers (SAMs) by measuring the localized surface plasmon resonance (LSPR) spectrum using UV−vis extinction spectroscopy. For all the experiments presented here, the Ag nanoparticles were fabricated using the technique of nanosphere lithography (NSL) and had in-plane widths of 100 nm and out-of-plane heights of 50 nm. We first demonstrate that unmodified nanoparticles are extremely susceptible to slight changes in 3-dimensional structure when exposed to various solvents. These structural effects can have dramatic effects on the extinction maximum, λ max, of the LSPR shifting it to the blue by over 100 nm. The significant discovery reported here is that λ max for NSL fabricated Ag nanoparticles is extremely sensitive to the SAM properties. We will demonstrate the following new features: (1) λ max of the LSPR linearly shifts to the red 3 nm for every carbon atom in the alkane chain; (2) spectral shifts as large as 40 nm are caused by only 60 000 alkanethiol molecules per nanoparticle, which corresponds to only 100 zmol of adsorbate; and (3) the nanoparticles' sensitivity to bulk external environment is only attenuated by 20% when the nanoparticles are modified with the longest chain alkanethiol (1-hexadecanethiol, ∼2 nm). Experimental extinction spectra were modeled by using Mie theory for Ag nanospheres with dielectric shells intended to mimic the self-assembled monolayer (SAM) in thickness and refractive index. We find that the Mie theory qualitatively predicts the experimentally observed trend that λ max linearly shifts to the red with respect to shell thickness, or alkanethiol chain length; however, the theory underestimates the sensitivity by approximately a factor of 4. Excellent correlation between theory and experiment was observed when Mie theory was used to predict the degree of attenuation in LSPR sensitivity to bulk external environment when the nanoparticle is encapsulated in a dielectric shell similar to an alkanethiol SAM. Finally, we demonstrate that Ag nanoparticles modified with functionalized SAMs can be used in sensing applications. Here, we show that the LSPR shifts to the red 5 nm with the adsorption of the polypeptide poly- l -lysine (PL) to Ag nanoparticles modified with deprotonated carboxylate groups from 11-mercaptoundecanoic acid (11-MUA). Furthermore, we will show that this system behaves reversibly and exhibits no detectable nonspecific binding.

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Metadata

Authors
Malinsky, M. D., Kelly, K. L., Schatz, G. C., & Van Duyne, R. P.
Venue
Journal of the American Chemical Society
Publisher
American Chemical Society (ACS)
Published
2001-01-30
Volume
123
Issue
7
Pages
1471-1482
ISSN
  • 0002-7863 (ISSN-L)
  • 1520-5126
DOI
10.1021/ja003312a
OpenAlex
W2056177922
Cited by
1,078
References
54
FWCI
23.74
Type
journal article
Language
en
Open access
closed

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