Orientation distributions of vacuum-deposited organic emitters revealed by single-molecule microscopy.

The orientation of luminescent molecules in organic light-emitting diodes strongly influences device performance. However, our understanding of the factors controlling emitter orientation is limited as current measurements only provide ensemble-averaged orientation values. Here, we use single-molecule imaging to measure the transition dipole orientation of individual emitter molecules in a state-of-the-art thermally evaporated host and thereby obtain complete orientation distributions of the hyperfluorescence-terminal emitter C545T.

Electroluminescence Generation in PbS Quantum Dot Light-Emitting Field-Effect Transistors with Solid-State Gating.

The application of light-emitting field-effect transistors (LEFET) is an elegant way of combining electrical switching and light emission in a single device architecture instead of two. This allows for a higher degree of miniaturization and integration in future optoelectronic applications. Here, we report on a LEFET based on lead sulfide quantum dots processed from solution.

Radiative Pumping and Propagation of Plexcitons in Diffractive Plasmonic Crystals.

Strong coupling between plasmons and excitons leads to the formation of plexcitons: quasiparticles that combine nanoscale energy confinement and pronounced optical nonlinearities. In addition to these localized modes, the enhanced control over the dispersion relation of propagating plexcitons may enable coherent and collective coupling of distant emitters. Here, we experimentally demonstrate strong coupling between carbon nanotube excitons and spatially extended plasmonic modes formed via diffractive coupling of periodically arranged gold nanoparticles (nanodisks, nanorods).

Trion-Polariton Formation in Single-Walled Carbon Nanotube Microcavities.

We demonstrate the formation and tuning of charged trion-polaritons in polymer-sorted (6,5) single-walled carbon nanotubes in a planar metal-clad microcavity at room temperature. The positively charged trion-polaritons were induced by electrochemical doping and characterized by angle-resolved reflectance and photoluminescence spectroscopy. The doping level of the nanotubes within the microcavity was controlled by the applied bias and thus enabled tuning from mainly excitonic to a mixture of exciton and trion transitions.

From Broadband to Electrochromic Notch Filters with Printed Monochiral Carbon Nanotubes.

Dense layers of semiconducting single-walled carbon nanotubes (SWNTs) serve as electrochromic (EC) materials in the near-infrared with high optical density and high conductivity. EC cells with tunable notch filter properties instead of broadband absorption are created via highly selective dispersion of specific semiconducting SWNTs through polymer-wrapping followed by deposition of thick films by aerosol-jet printing. A simple planar geometry with spray-coated mixed SWNTs as the counter electrode renders transparent metal oxides redundant and facilitates complete bleaching within a few seconds through iongel electrolytes with high ionic conductivities.

Infrared Organic Light-Emitting Diodes with Carbon Nanotube Emitters.

While organic light-emitting diodes (OLEDs) covering all colors of the visible spectrum are widespread, suitable organic emitter materials in the near-infrared (nIR) beyond 800 nm are still lacking. Here, the first OLED based on single-walled carbon nanotubes (SWCNTs) as the emitter is demonstrated. By using a multilayer stacked architecture with matching charge blocking and charge-transport layers, narrow-band electroluminescence at wavelengths between 1000 and 1200 nm is achieved, with spectral features characteristic of excitonic and trionic emission of the employed (6,5) SWCNTs.

Multispectral electroluminescence enhancement of single-walled carbon nanotubes coupled to periodic nanodisk arrays.

The integration of periodic nanodisk arrays into the channel of a light-emitting field-effect transistor leads to enhanced and directional electroluminescence from thin films of purified semiconducting single-walled carbon nanotubes. The maximum enhancement wavelength is tunable across the near-infrared and is directly linked to the periodicity of the arrays. Numerical calculations confirm the role of increased local electric fields in the observed emission modification.

Photocurrent spectroscopy of dye-sensitized carbon nanotubes.

Monochiral (7,5) single walled carbon nanotubes (SWCNTs) are integrated into a field effect transistor device in which the built-in electric field at the nanotube/metal contact allows for exciton separation under illumination. Variable wavelength spectroscopy and 2D surface mapping of devices consisting of 10-20 nanotubes are performed in the visible region and a strong correlation between the nanotube's second optical transition (S) and the photocurrent is found. After integration, the SWCNTs are non-covalently modified with three different fluorescent dye molecules with off-resonant absorption maxima at 532 nm, 565 nm, and 610 nm.

Electrical pumping and tuning of exciton-polaritons in carbon nanotube microcavities.

Exciton-polaritons are hybrid light-matter particles that form upon strong coupling of an excitonic transition to a cavity mode. As bosons, polaritons can form condensates with coherent laser-like emission. For organic materials, optically pumped condensation was achieved at room temperature but electrically pumped condensation remains elusive due to insufficient polariton densities.

Fitting Single-Walled Carbon Nanotube Optical Spectra.

In this work, a comprehensive methodology for the fitting of single-walled carbon nanotube absorption spectra is presented. Different approaches to background subtraction, choice of line profile, and calculation of full width at half-maximum are discussed both in the context of previous literature and the contemporary understanding of carbon nanotube photophysics. The fitting is improved by the inclusion of exciton-phonon sidebands, and new techniques to improve the individualization of overlapped nanotube spectra by exploiting correlations between the first- and second-order optical transitions and the exciton-phonon sidebands are presented.

Surface Lattice Resonances for Enhanced and Directional Electroluminescence at High Current Densities.

Hybrid photonic-plasmonic modes in periodic arrays of metallic nanostructures offer a promising trade-off between high-quality cavities and subdiffraction mode confinement. However, their application in electrically driven light-emitting devices is hindered by their sensitivity to the surrounding environment and to charge injecting metallic electrodes in particular. Here, we demonstrate that the planar structure of light-emitting field-effect transistor (LEFET) ensures undisturbed operation of the characteristic modes.

Near-infrared exciton-polaritons in strongly coupled single-walled carbon nanotube microcavities.

Exciton-polaritons form upon strong coupling between electronic excitations of a material and photonic states of a surrounding microcavity. In organic semiconductors the special nature of excited states leads to particularly strong coupling and facilitates condensation of exciton-polaritons at room temperature, which may lead to electrically pumped organic polariton lasers. However, charge carrier mobility and photo-stability in currently used materials is limited and exciton-polariton emission so far has been restricted to visible wavelengths.

Plasmonic Crystals for Strong Light-Matter Coupling in Carbon Nanotubes.

Their high oscillator strength and large exciton binding energies make single-walled carbon nanotubes (SWCNTs) highly promising materials for the investigation of strong light-matter interactions in the near infrared and at room temperature. To explore their full potential, high-quality cavities-possibly with nanoscale field localization-are required. Here, we demonstrate the room temperature formation of plasmon-exciton polaritons in monochiral (6,5) SWCNTs coupled to the subdiffraction nanocavities of a plasmonic crystal created by a periodic gold nanodisk array.

Broadband Tunable, Polarization-Selective and Directional Emission of (6,5) Carbon Nanotubes Coupled to Plasmonic Crystals.

We demonstrate broadband tunability of light emission from dense (6,5) single-walled carbon nanotube thin films via efficient coupling to periodic arrays of gold nanodisks that support surface lattice resonances (SLRs). We thus eliminate the need to select single-walled carbon nanotubes (SWNTs) with different chiralities to obtain narrow linewidth emission at specific near-infrared wavelengths. Emission from these hybrid films is spectrally narrow (20-40 meV) yet broadly tunable (∼1000-1500 nm) and highly directional (divergence <1.