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Nanoantennas capable of large fluorescence enhancement with minimal absorption are crucial for future optical technologies from single-photon sources to biosensing. Efficient dielectric nanoantennas have been designed, however, evaluating their performance at the individual emitter level is challenging due to the complexity of combining high-resolution nanofabrication, spectroscopy and nanoscale positioning of the emitter. Here, we study the fluorescence enhancement in infinity-shaped gallium phosphide (GaP) nanoantennas based on a topologically optimized design. Using fluorescence correlation spectroscopy (FCS), we probe the nanoantennas enhancement factor and observe an average of 63-fold fluorescence brightness enhancement with a maximum of 93-fold for dye molecules in nanogaps between 20 and 50 nm. The experimentally determined fluorescence enhancement of the nanoantennas is confirmed by numerical simulations of the local density of optical states (LDOS). Furthermore, we show that beyond design optimization of dielectric nanoantennas, increased performances can be achieved via tailoring of nanoantenna fabrication.

Metal-oxide semiconductors (MOS) are widely utilized for catalytic and photocatalytic applications in which the dynamics of charged carriers (e.g., electrons, holes) play important roles. Under operation conditions, photoinduced surface oxygen vacancies (PI-SOV) can greatly impact the dynamics of charge carriers. However, current knowledge regarding the effect of PI-SOV on the dynamics of hole migration in MOS films, such as titanium dioxide, is solely based upon volume-averaged measurements and/or vacuum conditions. This limits the basic understanding of hole-vacancy interactions, as they are not capable of revealing time-resolved variations during operation. Here, we measured the effect of PI-SOV on the dynamics of hole migration using time-resolved atomic force microscopy. Our findings demonstrate that the time constant associated with hole migration is strongly affected by PI-SOV, in a reversible manner. These results will nucleate an insightful understanding of the physics of hole dynamics and thus enable emerging technologies, facilitated by engineering hole-vacancy interactions.

We propose a design concept for tailoring the local density of optical states (LDOS) in dielectric nanostructures, based on the phase distribution of the scattered optical fields induced by point-like emitters. First we demonstrate that the LDOS can be expressed in terms of a coherent summation of constructive and destructive contributions. By using an iterative approach, dielectric nanostructures can be designed to effectively remove the destructive terms. In this way, dielectric Mie resonators, featuring low LDOS for electric dipoles, can be reshaped to enable enhancements of 3 orders of magnitude. To demonstrate the generality of the method, we also design nanocavities that enhance the radiated power of a circular dipole, a quadrupole, and an arbitrary collection of coherent dipoles. Our concept provides a powerful tool for high-performance dielectric resonators and affords fundamental insights into light-matter coupling at the nanoscale.

Quantum emitters radiate light omni-directionally, making it hard to collect and use the generated photons. Here, we propose a three-dimensional metal-dielectric parabolic antenna surrounding an individual quantum dot as a source of collimated single photons, which can then be easily extracted and manipulated. Our fabrication method relies on a single optically induced polymerization step once the selected emitter has been localized by confocal microscopy. Compared to conventional nanoantennas, our geometry does not require near-field coupling, and it is, therefore, very robust against misalignment issues and minimally affected by absorption in the metal. The parabolic antenna provides one of the largest reported experimental directivities ( D = 106) and the lowest beam divergences (Θ 1/2 = 13.5°) and a broadband operation over all of the visible and near-infrared range together with extraction efficiency of more than 96%, offering a practical advantage for quantum technological applications.

Resonant optical antennas are ideal for nanoscale nonlinear optical interactions due to their inherent strong local field enhancement. Indeed second- and third-order nonlinear response of gold nanoparticles has been reported. Here we compare the on- and off-resonance properties of aluminum, silver, and gold nanoantennas, by measuring two-photon photoluminescence. Remarkably, aluminum shows 2 orders of magnitude higher luminescence efficiency than silver or gold. Moreover, in striking contrast to gold, the aluminum emission largely preserves the linear incident polarization. Finally, we show the systematic resonance control of two-photon excitation and luminescence polarization by tuning the antenna width and length independently. Our findings point to aluminum as a promising metal for nonlinear plasmonics.