Herein, we present the use of a single gold nanorod sensor for detection of diseases on an antibody-functionalized surface, based on antibody-antigen interaction and the localized surface plasmon resonance (LSPR) λ(max) shifts of the resonant Rayleigh light scattering spectra. By replacing the cetyltrimethylammonium bromide (CTAB), a tightly packed self-assembled monolayer of HS(CH(2))(11)(OCH(2)CH(2))(6)OCH(2)COOH(OEG(6)) has been successfully formed on the gold nanorod surface prior to the LSPR sensing, leading to the successful fabrication of individual gold nanorod immunosensors. Using prostate specific antigen (PSA) as a protein biomarker, the lowest concentration experimentally detected was as low as 111 aM, corresponding to a 2.79 nm LSPR λ(max) shift. These results indicate that the detection platform is very sensitive and outperforms detection limits of commercial tests for PSA so far. Correlatively, its detection limit can be equally compared to the assays based on DNA biobarcodes. This study shows that a gold nanorod has been used as a single nanobiosensor to detect antigens for the first time; and the detection method based on the resonant Rayleigh scattering spectrum of individual gold nanorods enables a simple, label-free detection with ultrahigh sensitivity.

Scientific interest in nanotechnology is driven by the unique and novel properties of nanometer-sized metallic materials such as the strong interaction between the conductive electrons of the nanoparticles and the incident light, caused by localized surface plasmon resonances (LSPRs). In this article, we analysed the relationship of the Rayleigh scattering properties of a single Au nanoparticle with its size, shape, and local dielectric environment. We also provided a detailed study on the refractive index sensitivity of three types of differently shaped Au nanoparticles, which were nanospheres, oval-shaped nanoparticles and nanorods. This study helps one to differentiate the Rayleigh light scattering from individual nanoparticles of different sizes and/or shapes and precisely obtain quantitative data as well as the correlated optical spectra of single gold nanoparticles from the inherently inhomogeneous solution of nanoparticles. These results suggest that the shape, size and aspect ratio of Au nanoparticles are important structural factors in determining the resonant Rayleigh light scattering properties of a single Au nanoparticle such as its spectral peak position, scattering-cross-section and refractive index sensitivity, which gives a handle for the choice of gold nanoparticles for the design and fabrication of single nanosensors.

We report a simple, ultra-sensitive, and straightforward method for non-labeling detection of a cancer biomarker, using Rayleigh light scattering spectroscopy of the individual nanosensor based on antibody-antigen recognition and localized surface plasmon resonance (LSPR) λ(max) shifts. By experimentally measuring the refractive index sensitivity of Au nanorods, the Au nanorod with an aspect ratio of ~3.5 was proven optimal for the LSPR sensing. To reduce the steric hindrance effect as well as to immobilize a large amount of ligand on the nanoparticle surface, various mixtures containing different molar ratios of HS(CH(2))(11)(OCH(2)CH(2))(6)OCH(2)COOH and HS(CH(2))(11)(OCH(2)CH(2))(3)OH were applied to form different self-assembled monolayer surfaces. The results showed that the best molar ratio for antibody conjugation was 1 : 10. When using individual Au nanorod sensors for the detection of prostate specific antigen (PSA), the lowest concentration recorded was ~1 aM (~6 × 10(5) molecules), corresponding to LSPR λ(max) shifts of ~4.2 nm. These results indicate that sensor miniaturization down to the nanoscale level, the reduction of steric hindrance, and optimization of size, shape, and aspect ratio of nanorods have led to a significant improvement in the detection limit of sensors.

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A strategy for attomolar-level detection of small molecule-size proteins is reported based on Rayleigh light scattering spectroscopy of individual nanoplasmonic aptasensors by exploiting the outstanding characteristics of gold colloids to amplify the nontransparent resonant signal at ultralow analyte concentrations. The fabrication method utilizes thiol-mediated adsorption of a DNA aptamer on the immobilized Au nanoparticle surface, the interfacial binding characteristics of the aptamer with its target molecules, and the antibody-antigen interaction through plasmonic resonance coupling of the Au nanoparticles. Using lysozyme as a model analyte for disease detection, the detection limit of the aptasensor is ∼7 × 10(3) aM, corresponding to the LSPR λmax shift of ∼2.25 nm. Up to a 380% increase in the localized resonant λmax shift is demonstrated upon antibody binding to the analyte compared to the primary response during signal amplification using immunogold colloids. This enhancement leads to a limit of detection of ∼7 aM, which is an improvement of three orders of magnitude. The results demonstrate substantial promise for developing coupled plasmonic nanostructures for ultrasensitive detection of various biological and chemical analytes.