Gleb M. Akselrod

Ultrafast spontaneous emission source using plasmonic nanoantennas

Typical emitters such as molecules, quantum dots and semiconductor quantum wells have slow spontaneous emission with lifetimes of 1–10 ns, creating a mismatch with high-speed nanoscale optoelectronic devices such as light-emitting diodes, single-photon sources and lasers. Here we experimentally demonstrate an ultrafast (<11 ps) yet efficient source of spontaneous emission, corresponding to an emission rate exceeding 90 GHz, using a hybrid structure of single plasmonic nanopatch antennas coupled to colloidal quantum dots. The antennas consist of silver nanocubes coupled to a gold film separated by a thin polymer spacer layer and colloidal core–shell quantum dots, a stable and technologically relevant emitter. We show an increase in the spontaneous emission rate of a factor of 880 and simultaneously a 2,300-fold enhancement in the total fluorescence intensity, which indicates a high radiative quantum efficiency of ∼50%. The nanopatch antenna geometry can be tuned from the visible to the near infrared, providing a promising approach for nanophotonics based on ultrafast spontaneous emission.

Visualization of exciton transport in ordered and disordered molecular solids

Transport of nanoscale energy in the form of excitons is at the core of photosynthesis and the operation of a wide range of nanostructured optoelectronic devices such as solar cells, light-emitting diodes and excitonic transistors. Of particular importance is the relationship between exciton transport and nanoscale disorder, the defining characteristic of molecular and nanostructured materials. Here we report a spatial, temporal and spectral visualization of exciton transport in molecular crystals and disordered thin films. Using tetracene as an archetype molecular crystal, the imaging reveals that exciton transport occurs by random walk diffusion, with a transition to subdiffusion as excitons become trapped. By controlling the morphology of the thin film, we show that this transition to subdiffusive transport occurs at earlier times as disorder is increased. Our findings demonstrate that the mechanism of exciton transport depends strongly on the nanoscale morphology, which has wide implications for the design of excitonic materials and devices.

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 MoS2, a two-dimensional semiconductor, into the colloidally synthesized nanocavities. We observe a 2000-fold enhancement in the PL intensity of MoS2--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.

Ultrafast Room-Temperature Single Photon Emission from Quantum Dots Coupled to Plasmonic Nanocavities

Efficient and bright single photon sources at room temperature are critical components for quantum information systems such as quantum key distribution, quantum state teleportation, and quantum computation. However, the intrinsic radiative lifetime of quantum emitters is typically ∼10 ns, which severely limits the maximum single photon emission rate and thus entanglement rates. Here, we demonstrate the regime of ultrafast spontaneous emission (∼10 ps) from a single quantum emitter coupled to a plasmonic nanocavity at room temperature. The nanocavity integrated with a single colloidal semiconductor quantum dot produces a 540-fold decrease in the emission lifetime and a simultaneous 1900-fold increase in the total emission intensity. At the same time, the nanocavity acts as a highly efficient optical antenna directing the emission into a single lobe normal to the surface. This plasmonic platform is a versatile geometry into which a variety of other quantum emitters, such as crystal color centers, can be integrated for directional, room-temperature single photon emission rates exceeding 80 GHz.

Trion-Induced Negative Photoconductivity in Monolayer MoS 2

Optical excitation typically enhances electrical conduction and low-frequency radiation absorption in semiconductors. We, however, observe a pronounced transient decrease of conductivity in doped monolayer molybdenum disulfide (MoS(2)), a two-dimensional (2D) semiconductor, using ultrafast optical-pump terahertz-probe spectroscopy. In particular, the conductivity is reduced to only 30% of its equilibrium value at high pump fluence. This anomalous phenomenon arises from the strong many-body interactions in the 2D system, where photoexcited electron-hole pairs join the doping-induced charges to form trions, bound states of two electrons and one hole. The resultant increase of the carrier effective mass substantially diminishes the conductivity.

Subdiffusive Exciton Transport in Quantum Dot Solids

Colloidal quantum dots (QDs) are promising materials for use in solar cells, light-emitting diodes, lasers, and photodetectors, but the mechanism and length of exciton transport in QD materials is not well understood. We use time-resolved optical microscopy to spatially visualize exciton transport in CdSe/ZnCdS core/shell QD assemblies. We find that the exciton diffusion length, which exceeds 30 nm in some cases, can be tuned by adjusting the inorganic shell thickness and organic ligand length, offering a powerful strategy for controlling exciton movement. Moreover, we show experimentally and through kinetic Monte Carlo simulations that exciton diffusion in QD solids does not occur by a random-walk process; instead, energetic disorder within the inhomogeneously broadened ensemble causes the exciton diffusivity to decrease over time. These findings reveal new insights into exciton dynamics in disordered systems and demonstrate the flexibility of QD materials for photonic and optoelectronic applications.

Large-Area Metasurface Perfect Absorbers from Visible to Near-Infrared.

An absorptive metasurface based on film-coupled colloidal silver nanocubes is demonstrated. The metasurfaces are fabricated using simple dip-coating methods and can be deposited over large areas and on arbitrarily shaped objects. The surfaces show nearly complete absorption, good off-angle performance, and the resonance can be tuned from the visible to the near-infrared.

Photon arrival time quantum random number generation

We present an efficient random number generator based on the randomness present in photon emission and detection. The interval between successive photons from a light source with Poissonian statistics is separated into individual time bins, which are then used to create several random bits per detection event. Using a single-photon counter and FPGA-based data processing allows for a cost-efficient and convenient implementation that outputs data at rates of roughly 40 Mbit s−1.

Cryogenic ion trapping systems with surface-electrode traps.

We present two simple cryogenic rf ion trap systems in which cryogenic temperatures and ultra high vacuum pressures can be reached in as little as 12 h. The ion traps are operated either in a liquid helium bath cryostat or in a low vibration closed cycle cryostat. The fast turn around time and availability of buffer gas cooling made the systems ideal for testing surface-electrode ion traps. The vibration amplitude of the closed cycled cryostat was found to be below 106 nm. We evaluated the systems by loading surface-electrode ion traps with (88)Sr(+) ions using laser ablation, which is compatible with the cryogenic environment. Using Doppler cooling we observed small ion crystals in which optically resolved ions have a trapped lifetime over 2500 min.

Twenty-Fold Enhancement of Molecular Fluorescence by Coupling to a J-Aggregate Critically Coupled Resonator

We report a 20-fold enhancement in the fluorescence of the organic dye DCM when resonantly coupled to a strongly optically absorbing structure of a thin film of spin-deposited molecular J-aggregates in a critically coupled resonator (JCCR) geometry. A submonolayer equivalent of DCM molecules is shown to absorb and re-emit 2.2% of the incident resonant photons when coupled to the JCCR enhancement structure, compared to 0.1% for the bare film of same thickness on quartz. Such a JCCR structure is a general energy focusing platform that localizes over 90% of incident light energy within a 15 nm thin film layer in the form of excitons that can subsequently be transferred to colocated lumophores. Applications of the exciton-mediated concentration of optical energy are discussed in the context of solid-state lighting, photodetection, and single photon optics.