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Shedding light on the extinction-enhancement duality in gold nanostar-enhanced Raman spectroscopy.

ABSTRACT: Surface-enhanced Raman spectroscopy (SERS) has evolved from an esoteric physical phenomenon to a robust and effective analytical method recently. The need of addressing both the field enhancement and the extinction of nanoparticle suspensions, however, has been underappreciated despite its substantive impact on the sensing performance. A systematic experimental investigation of SERS enhancement and attenuation is performed in suspensions of gold nanostars, which exhibit a markedly different behavior in relation to conventional nanoparticles. The relationship is elucidated between the SERS enhancement and the localized surface plasmon resonance band, and the effect of the concentration of the gold nanostars on the signal propagation is investigated. It is shown that an optimal concentration of gold nanostars exists to maximize the enhancement factor (EF), and the maximum EF occurs when the LSPR band is blue-shifted from the excitation wavelength rather than at the on-resonance position.

SUBMITTER: Li M

PROVIDER: S-EPMC4294795 | biostudies-literature | 2014 Dec

REPOSITORIES: biostudies-literature

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Shedding light on the extinction-enhancement duality in gold nanostar-enhanced Raman spectroscopy.

Li Ming M Kang Jeon Woong JW Dasari Ramachandra Rao RR Barman Ishan I

Angewandte Chemie (International ed. in English) 20141021 51

Surface-enhanced Raman spectroscopy (SERS) has evolved from an esoteric physical phenomenon to a robust and effective analytical method recently. The need of addressing both the field enhancement and the extinction of nanoparticle suspensions, however, has been underappreciated despite its substantive impact on the sensing performance. A systematic experimental investigation of SERS enhancement and attenuation is performed in suspensions of gold nanostars, which exhibit a markedly different beha ...[more]

PMID: 25331156

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Project description:The plasmonic properties of carboxylated gold nanostars distributed on amidoximated polyacrylonitrile (AO PAN) electrospun polymer films scale with surface-enhanced Raman scattering (SERS) intensities for coordinated uranium(VI) oxide (uranyl) species. This two-step plasmonic sensor first isolates uranyl from solution using functionalized polymers; then carboxylated gold nanostars are subsequently deposited for SERS. Spatially resolved localized surface plasmon resonance (LSPR) and SERS facilitate correlated nanostar optical density and uranyl quantification. To reduce sampling bias, gold nanostars are deposited in an inverted drop-coating geometry and measurements are conducted inside resulting nanoparticle coffee rings that form on the polymer substrates. This approach naturally preserves the plasmonic properties of gold nanostars while reducing the deposition of nanoparticle aggregates in active sensing regions, thereby maximizing both the accuracy and the precision of SERS measurements. Several advances are made. First, second-derivative analysis of LSPR spectra facilitates the quantification of local nanostar density across large regions of the sensor substrate by reducing background variations caused by the polymeric and gold materials. Second, local nanostar densities ranging from 140 to 200 pM·cm are shown to result in uranyl signals that are independent of nanostar concentration. Third, the Gibbs free energy of uranyl adsorption to carboxylated nanostars is estimated at 8.4 ± 0.2 kcal/mol. Finally, a linear dynamic range from ∼0.3 to 3.4 μg U/mg polymer is demonstrated. Signals vary by 10% or less. As such, the uniformity of the plasmonic activity of distributed gold nanostars and the employment of spatially resolved spectroscopic measurements on the composite nanomaterial sensor interface facilitate the quantitative detection of uranyl while also reducing the dependence on user expertise and the selected sampling region. These important advances are critical for the development of a user-friendly SERS-based sensor for uranyl.

Dataset Information

Shedding light on the extinction-enhancement duality in gold nanostar-enhanced Raman spectroscopy.

Publications

Shedding light on the extinction-enhancement duality in gold nanostar-enhanced Raman spectroscopy.

Similar Datasets

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