Plasmonic antennas have a profound impact on nanophotonics as they provide efficient means to manipulate light and enhance light-matter interactions at the nanoscale. However, the large absorption losses found in metals can severely limit the plasmonic applications in the visible spectral range. Here, we demonstrate the effectiveness of an alternative approach using all-dielectric nanoantennas based on silicon dimers to enhance the fluorescence detection of single molecules. The silicon antenna design is optimized to confine the near-field intensity in the 20 nm nanogap and reach a 270-fold fluorescence enhancement in a nanoscale volume of λ(3)/1800 with dielectric materials only. Our conclusions are assessed by combining polarization resolved optical spectroscopy of individual antennas, scanning electron microscopy, numerical simulations, fluorescence lifetime measurements, fluorescence burst analysis, and fluorescence correlation spectroscopy. This work demonstrates that all-silicon nanoantennas are a valid alternative to plasmonic devices for enhanced single molecule fluorescence sensing, with the additional key advantages of reduced nonradiative quenching, negligible heat generation, cost-efficiency, and complementary metal-oxide-semiconductor (CMOS) compatibility.
Frequency conversion is one of the main applications of nonlinear optical processes in which a signal is produced at a different wavelength from the excitation wavelength.In particular, four-wave mixing (FWM) is a third order non-linear optical process that allows, for instance, the generation of visible frequencies by tuning near-infrared laser pumps. Here, in order to augment the very weak FWM conversion efficiency, we design silicon Mie resonators that exhibit two resonances of the internal electric field intensity 1 around the frequency range of the laser pumps. The linear extinction spectrum of the individual Si resonator is first measured by bright field spectroscopy and compared with numerical simulations to confirm the existence of the two resonances corresponding to electric and magnetic dipoles excitations. The FWM signal is then measured for a single Si nanoresonator when the first pump is set to the electric resonance, while tuning the frequency of the second pump across the magnetic dipolar resonance. We show that the FWM signal generated in the visible spectrum is maximum when the frequency of the tunable pump corresponds to the maximum of the internal electric field intensity.At this position, the FWM signal is enhanced by more than two orders of magnitude compared with the FWM signal generated by the unpatterned silicon film.
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