Leveraging Nanocavity Harmonics for Control of Optical Processes in 2D Semiconductors

Optical cavities with multiple tunable resonances have the potential to provide unique electromagnetic environments at two or more distinct wavelengths—critical for control of optical processes such as nonlinear generation, entangled photon generation, or photoluminescence (PL) enhancement. Here, we show a plasmonic nanocavity based on a nanopatch antenna design that has two tunable resonant modes in the visible spectrum separated by 350 nm and with line widths of ∼60 nm. The importance of utilizing two resonances simultaneously is demonstrated by integrating monolayer MoS[subscript 2], a two-dimensional semiconductor, into the colloidally synthesized nanocavities. We observe a 2000-fold enhancement in the PL intensity of MoS[subscript 2]—which has intrinsically low absorption and small quantum yield—at room temperature, enabled by the combination of tailored absorption enhancement at the first harmonic and PL quantum-yield enhancement at the fundamental resonance.United States. Dept. of Energy. Center for Excitonics (Award DE-SC0001088)United States. Dept. of Energy. Office of Basic Energy Sciences (Grant DE-SC0001088

Widely tunable, efficient on-chip single photon sources at telecommunication wavelengths

We demonstrate tunable on-chip single photon sources using the Stark tuning of single quantum dot (QD) excitonic transitions in short photonic crystal waveguides (PhC WGs). The emission of single QDs can be tuned in real-time by 9 nm with an applied bias voltage less than 2V. Due to a reshaped density of optical modes in the PhC WG, a large coupling efficiency \beta>65% to the waveguide mode is maintained across a wavelength range of 5 nm. When the QD is resonant with the Fabry-Perot mode of the PhC WG, a strong enhancement of spontaneous emission is observed leading to a maximum coupling efficiency \beta=88%. These results represent an important step towards the scalable integration of single photon sources in quantum photonic integrated circuits.Comment: 15 pages, 5 figue

Ultrafast nonlocal control of spontaneous emission

Solid-state cavity quantum electrodynamics systems will form scalable nodes of future quantum networks, allowing the storage, processing and retrieval of quantum bits, where a real-time control of the radiative interaction in the cavity is required to achieve high efficiency. We demonstrate here the dynamic molding of the vacuum field in a coupled-cavity system to achieve the ultrafast nonlocal modulation of spontaneous emission of quantum dots in photonic crystal cavities, on a timescale of ~200 ps, much faster than their natural radiative lifetimes. This opens the way to the ultrafast control of semiconductor-based cavity quantum electrodynamics systems for application in quantum interfaces and to a new class of ultrafast lasers based on nano-photonic cavities.Comment: 15 pages, 4 figure

Growth, Structural and Optical Properties of High Quality GaAs Nanowires for Optoelectronics

We investigate how growth parameters may be chosen to obtain high quality GaAs nanowires suitable for optoelectronic device applications. Growth temperature and precursor flows have a significant effect on the morphology, crystallographic quality, intrinsic doping and optical properties of the resulting nanowires. Significantly, we find that low growth temperature and high arsine flow rate improve nanowire optical properties, reduce carbon impurity incorporation and drastically reduce planar crystallographic defects. Additionally, cladding the GaAs nanowire cores in an AlGaAs shell enhances emission efficiency. These high quality nanowires should create new opportunities for optoelectronic devices

Broad electrical tuning of plasmonic nanoantennas at visible frequencies

We report an experimental demonstration of electrical tuning of plasmon resonances of optical nanopatch antennas over a wide wavelength range. The antennas consist of silver nanocubes separated from a gold film by a thin 8 nm polyelectrolyte spacer layer. By using ionic liquid and indium tin oxide coated glass as a top electrode, we demonstrate dynamic and reversible tuning of the plasmon resonance over 100 nm in the visible wavelength range using low applied voltages between -3.0 V and 2.8 V. The electrical potential is applied across the nanoscale gap causing changes in the gap thickness and dielectric environment which, in turn, modifies the plasmon resonance. The observed tuning range is greater than the full-width-at-half-maximum of the plasmon resonance, resulting in a tuning figure of merit of 1.05 and a tuning contrast greater than 50%. Our results provide an avenue to create active and reconfigurable integrated nanophotonic components for applications in optoelectronics and sensing

Fast spontaneous emission and high Förster resonance energy transfer rate in hybrid organic/inorganic plasmonic nanostructures

We report an experimental study of the plasmon-assisted spontaneous emission and the Förster resonance energy transfer between organic molecules and semiconductor colloidal quantum dots. The localized plasmonic field in the nanogap between a gold nano-popcorn\u27s tips and a 5-nm separated gold film supports high photonic density of states and provides pathways for the light-matter interaction mechanisms. We demonstrate that, besides the total enhanced decay rate up to 66 times for quantum dots and molecules, the Förster resonance energy transfer efficiency and rate constant are simultaneously modified. While the energy transfer efficiency is reduced from 84% to 35% due to the non-radiative quenching effect and fast donor decay rate, the energy transfer rate constant is significantly increased from 4 to 20 ns-1. Our results have quantitatively elucidated decay mechanisms that are important toward understanding and controlling of the light-matter interaction at the nanoscale