Near- and far-field study of polarization-dependent surface plasmon resonance in bowtie nano-aperture arrays.

Bowtie nano-apertures can confine light into deep subwavelength volumes with extreme field enhancement, making them a useful tool for various applications such as optical trapping, deep subwavelength imaging, nanolithography, and sensors. However, the correlation between the near- and far-field properties of bowtie nano-aperture arrays has yet to be fully explored. In this study, we experimentally investigated the polarization-dependent surface plasmon resonance in bowtie nano-aperture arrays using both optical transmission spectroscopy and photoemission electron microscopy. The experimental results reveal a nonlinear redshift in the transmission spectra as the gap size of the bowtie nanoaperture decreases for vertically polarized light, while the transmission spectra remain unchanged with different gap sizes for horizontally polarized light. To elucidate the underlying mechanisms, we present simulated charge and current distributions, revealing how the electrons respond to light and generate the plasmonic fields. These near-field distributions were verified by photoemission electron microscopy. This study provides a comprehensive understanding of the plasmonic properties of bowtie nano-aperture, enabling their further applications, one of which is the optical switching of the resonance wavelength in the widely used visible spectral region without changing the geometry of the nanostructure.

Surface-Plasmonic-Field-Induced Photoredox Catalysis and Mediated Electron Transfer for Washing-Free DNA Detection.

Distance-dependent electromagnetic radiation and electron transfer have been commonly employed in washing-free fluorescence and electrochemical bioassays, respectively. In this study, we combined the two distance-dependent phenomena for sensitive washing-free DNA detection. A distance-dependent surface plasmonic field induces rapid photoredox catalysis of surface-bound catalytic labels, and distance-dependent mediated electron transfer allows for rapid electron transfer from the surface-bound labels to the electrode. An optimal system consists of a chemically reversible acceptor (Ru(NH3 )63+ ), a chemically reversible photoredox catalyst (eosin Y), and a chemically irreversible donor (triethanolamine). Side reactions with O2 do not significantly decrease the efficiency of photoredox catalysis. Energy transfer quenching between the electrode and the label can be lowered by increasing the distance between them. Washing-free DNA detection had a detection limit of approximately 0.3 nm in buffer and 0.4 nm in serum without a washing step.

Enhanced third harmonic generation in ultrathin free-standing ß-Ga2O3 nanomembranes: study on surface and bulk contribution.

Third harmonic generation (THG) has proven its value in surface and interface characterization, high-contrast bio-imaging, and sub-wavelength light manipulation. Although THG is observed widely in general solid and liquid substances, when laser pulses are focused at nanometer-level ultra-thin films, the bulk THG has been reported to play the dominant role. However, there are still third harmonics (TH) generated at the surface of the thin-films, not inside the bulk solid - so-called surface TH, whose relative contribution has not been quantitatively revealed to date. In this study, we quantitatively characterized the surface and bulk contributions of THG at ultra-thin ß-Ga2O3 nanomembranes with control of both the laser and thin-nanomembranes parameters, including the laser peak power, polarization state, number of layers, and nanomembranes thicknesses. Their contributions were studied in detail by analyzing the TH from freestanding ß-Ga2O3 nanomembranes compared with TH from ß-Ga2O3 nanomembranes on glass substrates. The contribution of the TH field from the ß-Ga2O3-air interface was found to be 5.12 times more efficient than that from the ß-Ga2O3-glass interface, and also 1.09 times stronger than the TH excited at bulk 1-µm-thick ß-Ga2O3. Besides, TH from the ß-Ga2O3-air interface was found to be 20% more sensitive to the crystalline structure than that from the ß-Ga2O3-glass interface. This research work deepens our understanding of surface and bulk THG from crystalline materials and provides new possibilities towards designing highly efficient nonlinear optical materials for bio-imaging, energy-harvesting, and ultrafast laser development.