Metallic Nanodroplet Induced Coulomb Catalysis for Off-Resonant Plasmonic Enhancement of Photoemission in Semiconductors.

The enhancement of light from semiconductors due to surface plasmons coupled resonantly to its emission is limited because of dissipation in the metal and is also restricted by the dielectric characteristics and homogeneity of the metal-semiconductor interface. We report a new mechanism based on electrostatic interactions of carriers and their image charges in metals to generate more photons from optical sources at frequencies that are off-resonant to the localized plasmon frequency. Coulomb catalysis of carrier accumulation resulting from the inhomogeneity of metal nanodroplets on a semiconductor's surface can result in an enhancement of light that is nondissipative and does not require resonant coupling of plasmons to the emission wavelength. The enhancement occurs because of an increase in the ratio of radiative to nonradiative recombination in the vicinity of metal nanoparticles. It is equally effective with any type of metal and enhances radiation at any frequency, a property that is of principal importance for the realization of widely tunable semiconductor emitters. This fundamental mechanism provides a new perspective for improving the efficiency of light emitters and controlling carrier concentration on the nanoscale. The structural characteristics of the hybrid metal-semiconductor emitters are studied using electron microscopy and atomic force microscopy. We demonstrate the electrostatic mechanism by studying steady-state and transient photoluminescence from two-dimensional semiconductors, such as GaAs/AlGAs quantum wells, and bulk semiconductors, such as ZnO thin films, emitting in the near-IR and UV wavelength regimes, respectively.