RESUMO
Confining photons in the smallest possible volume has long been an objective of the nanophotonics community. In this Letter, we propose and demonstrate a three-dimensional (3D) gap-plasmon antenna that enables extreme photon squeezing in a 3D fashion with a modal volume of 1.3 × 10(-7) λ(3) (â¼4 × 10 × 10 nm(3)) and an intensity enhancement of 400â¯000. A three-dimensionally tapered 4 nm air-gap is formed at the center of a complementary nanodiabolo structure by ion-milling 100 nm-thick gold film along all three dimensions using proximal milling techniques. From a 4 nm-gap antenna, a nonlinear second-harmonic signal more than 27â¯000-times stronger than that from a 100 nm-gap antenna is observed. In addition, scanning cathodoluminescence images confirm unambiguous photon confinement in a resolution-limited area 20 × 20 nm(2) on top of the nano gap.
RESUMO
Detection of single nanoparticles or molecules has often relied on fluorescent schemes. However, fluorescence detection approaches limit the range of investigable nanoparticles or molecules. Here, we propose and demonstrate a non-fluorescent nanoscopic trapping and monitoring platform that can trap a single sub-5-nm particle and monitor it with a pair of floating nonlinear point sources. The resonant photon funnelling into an extremely small volume of ~5 × 5 × 7 nm3 through the three-dimensionally tapered 5-nm-gap plasmonic nanoantenna enables the trapping of a 4-nm CdSe/ZnS quantum dot with low intensity of a 1560-nm continuous-wave laser, and the pumping of 1560-nm femtosecond laser pulses creates strong background-free second-harmonic point illumination sources at the two vertices of the nanoantenna. Under the stable trapping conditions, intermittent but intense nonlinear optical spikes are observed on top of the second-harmonic signal plateau, which is identified as the 3.0-Hz Kramers hopping of the quantum dot trapped in the 5-nm gap.