Jingyi Zhao

Surface enhanced fluorescence by metallic nano-apertures associated with stair-gratings

Metallic nano-apertures associated with stair-gratings are proposed for surface enhanced fluorescence with high excitation enhancement and narrow emission beaming effect. Fluorescence correlation spectroscopy method was utilized to analyze the fluorescence trace and fluorescence enhancement, and the angular patterns of fluorescent emission were measured with the back focal plane imaging method. The stair-grating presents a strong optical response which covering well both the excitation and the emission bands of the photoluminescence process. Such high enhancement and narrow directionality by the stair-gratings would enable the detection of single molecules with low numerical aperture objective effectively.

Nano-gap between a gold tip and nanorod for polarization dependent surface enhanced Raman scattering

We demonstrate experimentally that a nano-gap could be constructed by using a scanning probe microscope to allow a gold tip to approach a gold nanorod immobilized on a glass coverslip. The nano-gap can enhance Raman scattering of graphene sandwiched between the tip and the nanorod. The Raman intensity was strongly dependent on the incident light polarization. Here, linear, radial, azimuthal, and intermediate states between radial and azimuthal polarization were investigated and compared in detail. The maximum surface-enhanced Raman scattering effect of the nano-gap occurred for the intermediate states between the radial and azimuthal polarized light.

Light Emission from Plasmonic Nanostructures Enhanced with Fluorescent Nanodiamonds

In the surface-enhanced fluorescence (SEF) process, it is well known that the plasmonic nanostructure can enhance the light emission of fluorescent emitters. With the help of atomic force microscopy, a hybrid system consisting of a fluorescent nanodiamond and a gold nanoparticle was assembled step-by-step for in situ optical measurements. We demonstrate that fluorescent emitters can also enhance the light emission from gold nanoparticles which is judged through the intrinsic anti-Stokes emission owing to the nanostructures. The light emission intensity, spectral shape, and lifetime of the hybrid system were dependent on the coupling configuration. The interaction between gold nanoparticles and fluorescent emitter was modelled based on the concept of a quantised optical cavity by considering the nanodiamond and the nanoparticle as a two-level energy system and a nanoresonator, respectively. The theoretical calculations reveal that the dielectric antenna effect can enhance the local field felt by the nanoparticle, which contributes more to the light emission enhancement of the nanoparticles rather than the plasmonic coupling effect. The findings reveal that the SEF is a mutually enhancing process. This suggests the hybrid system should be considered as an entity to analyse and optimise surface-enhanced spectroscopy.

Understanding photoluminescence of metal nanostructures based on an oscillator model

Scattering and absorption properties of metal nanostructures have been well understood based on the classic oscillator theory. Here, we demonstrate that photoluminescence of metal nanostructures can also be explained based on a classic model. The model shows that inelastic radiation of an oscillator resembles its resonance band after external excitation, and is related to the photoluminescence from metallic nanostructures. The understanding based on the classic oscillator model is in agreement with that predicted by a quantum electromagnetic cavity model. Moreover, by correlating a two-temperature model and the electron distributions, we demonstrate that both one-photon and two-photon luminescence of the metal nanostructures undergo the same mechanism. Furthermore, the model explains most of the emission characteristics of the metallic nanostructures, such as quantum yield, spectral shape, excitation polarization and power dependence. The model based on an oscillator provides an intuitive description of the photoluminescence process and may enable rapid optimization and exploration of the plasmonic properties.

Hybrid Metal-Dielectric Nano-Aperture Antenna for Surface Enhanced Fluorescence

A hybrid metal-dielectric nano-aperture antenna is proposed for surface-enhanced fluorescence applications. The nano-apertures that formed in the composite thin film consist of silicon and gold layers. These were numerically investigated in detail. The hybrid nano-aperture shows a more uniform field distribution within the apertures and a higher antenna quantum yield than pure gold nano-apertures. The spectral features of the hybrid nano-apertures are independent of the aperture size. This shows a high enhancement effect in the near-infrared region. The nano-apertures with a dielectric gap were then demonstrated theoretically for larger enhancement effects. The hybrid nano-aperture is fully adaptable to large-scale availability and reproducible fabrication. The hybrid antenna will improve the effectiveness of surface-enhanced fluorescence for applications, including sensitive biosensing and fluorescence analysis.

Luminescence quantum yields of gold nanoparticles varying with excitation wavelength

Luminescence quantum yields (QYs) of gold nanoparticles including nanorods, nanobipyramids and nanospheres are measured elaborately at single nanoparticle level with different excitation wavelengths. It is found that the QYs of the nanostructures are essentially dependent on the excitation wavelength. The QY is higher when the excitation wavelength is blue-detuned and close to the nanoparticles’ surface plasmon resonant peak. A phenomenological model based on plasmonic resonator concept is proposed to understand the experimental findings. The excitation wavelength dependent of QY is attributed to the wavelength dependent coupling efficiency between the free electrons oscillation and the intrinsic plasmon resonant radiative mode. These studies should contribute to the understanding of one-photon luminescence from metallic nanostructures and plasmonic surface enhanced spectroscopy.

Spectral shape of one-photon luminescence from single gold nanorods

Light emission from gold nanoparticles was investigated with ultra-narrow-band notch filters to obtain the complete spectral shape. The anti-Stokes emission band was observed at all excitation wavelengths. The spectral shape of the anti-Stokes emission could be well fitted by a Fermi–Dirac-like line shape, while the spectral profile of the Stokes emission could be fitted by a Lorentzian line shape. The electron distribution and local surface plasmon resonance jointly determined the spectral shape. Additionally, we found that the anti-Stokes emission intensity increased more rapidly compared with that of the Stokes emission as illumination power was increased. This phenomenon can be understood from the temperature dependence of the electron distribution owing to photothermal effects.