No abstract

Abstract. Single walled carbon nanotubes (SWNTs) are luminescent. Up to now, two preparation methods, both of which isolate individual SWNTs, have enabled the detection of nanotube bandgap photoluminescence (PL): encapsulation of individual SWNTs into surfactant micelles, and direct growth of individual SWNTs suspended in air between pillars. This paper compares the PL obtained from suspended SWNTs to published PL data obtained from encapsulated SWNTs. We find that emission peaks are blue-shifted by 28 meV on average for the suspended nanotubes as compared to the encapsulated nanotubes. Similarly, the resonant absorption peaks are blue-shifted on average by 16 meV. Both shifts depend weakly on the particular chirality and diameter of the SWNT.

Single air-suspended carbon nanotubes (length 2-5 microm) exhibit high optical quantum efficiency (7-20%) for low intensity resonant pumping. Under ultrafast excitation (150 fs), emission dramatically saturates at very low exciton numbers (2-6), which is attributed to highly efficient exciton-exciton annihilation over micron-length scales. Similar saturation behavior for 4 ps pulse excitation shows nonlinear absorption is not a contributing factor. The absorption cross sections (0.6-1.8x10(-17) cm2/atom) are determined by fitting to a stochastic model for exciton dynamics.

In atomically thin two-dimensional semiconductors such as transition metal dichalcogenides (TMDs), controlling the density and type of defects promises to be an effective approach for engineering light-matter interactions. We demonstrate that electron-beam irradiation is a simple tool for selectively introducing defect-bound exciton states associated with chalcogen vacancies in TMDs. Our first-principles calculations and time-resolved spectroscopy measurements of monolayer WSe_{2} reveal that these defect-bound excitons exhibit exceptional optical properties including a recombination lifetime approaching 200 ns and a valley lifetime longer than 1  μs. The ability to engineer the crystal lattice through electron irradiation provides a new approach for tailoring the optical response of TMDs for photonics, quantum optics, and valleytronics applications.