Kai-Xin Xie

Label-free aptasensor based on ultrathin-linker-mediated hot-spot assembly to induce strong directional fluorescence.

We have demonstrated the proof-of-concept of a label-free biosensor based on emission induced by an extreme hot-spot plasmonic assembly. In this work, an ultrathin linking layer composed of cationic polymers and aptamers was fabricated to mediate the assembly of a silver nanoparticles (AgNPs)-dyes-gold film with a strongly coupled architecture through sensing a target protein. Generation of directional surface plasmon coupled emission (SPCE) was thus stimulated as a means of reporting biorecognition. Both the biomolecules and the nanoparticles were totally free of labeling, thereby ensuring the activity of biomolecules and allowing the use of freshly prepared metallic nanoparticles with large dimensions. This sensor smartly prevents the plasmonic assembly in the absence of targets, thus maintaining no signal through quenching fluorophores loaded onto a gold film. In the presence of targets, the ultrathin layer is activated to link NPs-film junctions. The small gap of the junction (no greater than 2 nm) and the large diameter of the nanoparticles (~100 nm) ensure that ultrastrong coupling is achieved to generate intense SPCE. A >500-fold enhancement of the signal was observed in the biosensing. This strategy provides a simple, reliable, and effective way to apply plasmonic nanostructures in the development of biosensing.

Surface Plasmon-Coupled Directional Enhanced Raman Scattering by Means of the Reverse Kretschmann Configuration

Surface-enhanced Raman scattering (SERS) is a unique analytical technique that provides fingerprint spectra, yet facing the obstacle of low collection efficiency. In this study, we demonstrated a simple approach to measure surface plasmon-coupled directional enhanced Raman scattering by means of the reverse Kretschmann configuration (RK-SPCR). Highly directional and p-polarized Raman scattering of 4-aminothiophenol (4-ATP) was observed on a nanoparticle-on-film substrate at 46° through the prism coupler with a sharp angle distribution (full width at half-maximum of ∼3.3°). Because of the improved collection efficiency, the Raman scattering signal was enhanced 30-fold over the conventional SERS mode; this was consistent with finite-difference time-domain simulations. The effect of nanoparticles on the coupling efficiency of propagated surface plasmons was investigated. Possessing straightforward implementation and directional enhancement of Raman scattering, RK-SPCR is anticipated to simplify SERS instruments and to be broadly applicable to biochemical assays.

Directional surface plasmon-coupled emission of CdTe quantum dots and its application in Hg(II) sensing

We investigated the surface plasmon-coupled emission (SPCE) of CdTe quantum dots (QDs) and developed an SPCE-based quenchometric sensor for Hg(II) ion sensing. CdTe QDs directly synthesized in aqueous solution were attached to a 50 nm-thick Au film through layer-by-layer assembly. The directional emission of the CdTe QDs on the prism side from the surface plasmon coupling was completely p-polarized and observed at a fixed angle of 48.5°, which was consistent with theoretical calculations. An SPCE-based quenchometric sensor for Hg(II) ion sensing was established based on the quenching effect of Hg(II) ions on the fluorescence emission of CdTe QDs. As expected, the SPCE-based sensor enlarged the response range and was more sensitive than that based on free-space detection as a result of the high light-collection efficiency of SPCE. QDs with excellent properties combined with SPCE technology have great potential in detecting analytes at low concentration levels.

Surface plasmon coupled emission in micrometer-scale cells: a leap from interface to bulk targets.

Surface plasmon coupled emission (SPCE) technique has attracted increasing attention in biomolecular interaction analysis and cell imaging because of its high sensitivity, low detection volume and low fluorescence background. Typically, the working range of SPCE is limited at nanometers to an interface. For micrometer-scale samples, new SPCE properties are expected because of complex coupling modes. In this work, cells with different subregions labeled were studied using a SPCE spectroscopy system. Angular and p-polarized emission was observed for cell membrane, cytoplasm, and nucleus labeled with DiI, Nile Red, and propidium iodide, respectively. The SPCE signals were always partially p-polarized, and the maximum emission angle did not shift, regardless of variations in emission wavelength, fluorophore distribution and stained layer thickness. Additionally, increased polarization and a broader angle distribution were also observed with an increase in sample thickness. We also investigated the impact of metallic substrates on the SPCE properties of cells. Compared with Au and Ni substrates, Al substrates presented better polarization and angle distribution. Moreover, the real-time detection of the cell labeling process was achieved by monitoring SPCE intensity. These findings expand SPCE from a surface technique to a 3D method for investigating bulk targets beyond the nanoscale interfaces, providing a basis to apply this technique to study cell membrane fluidity and biomolecule interactions inside the cell and to distinguish between cell subregions.

High performance dual-mode surface plasmon coupled emission imaging apparatus integrating Kretschmann and reverse Kretschmann configurations for flexible measurements

A Kretschmann (KR) and reverse Kretschmann (RK) dual-mode surface plasmon coupled emission (SPCE) imaging apparatus based on prism coupling was built up. Highly directional and polarized fluorescence images for both RK and KR configurations were obtained. Besides, surface plasmon field-enhanced fluorescence and free space imaging can also be measured conveniently from this apparatus. Combining the high sensitivity of KR mode and the simplicity of RK mode, the multifunctional imaging system is flexible to provide different configurations for imaging applications. Compared to the free space imaging, SPCE imaging provides enhanced fluorescence, especially large enhancement up to about 50 fold in KR configuration. Additionally, the degree of evanescent field enhancement effect was easily estimated experimentally using the apparatus to compare the different imaging configurations. We believed that the dual-mode SPCE imaging apparatus will be useful in fundamental study of plasmon-controlled fluorescence and be a powerful tool for optical imaging, especially for microarray and biological applications.

Optical modulator based on propagating surface plasmon coupled fluorescent thin film: proof-of-concept studies

We demonstrate that the propagating surface plasmon coupled fluorescent thin film can be utilized as a fluorescence modulator to mimic multiple representative Boolean logic operations. Surface plasmon mediated fluorescence presents characteristic properties including directional and polarized emission, which hold the feasibility in creating a universal optical modulator. In this work, through constructing the thin layer with the specific thickness, surface plasmon mediated fluorescence can be modulated with an ON-OFF ratio by more than 5-fold, under a series of coupling configurations.