Arko Graf

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 <1.5°). In addition, SLR scattering renders the emission highly polarized, even though the SWNTs are randomly distributed. Numerical simulations are applied to correlate the increased local electric fields around the nanodisks with the observed enhancement of directional emission. The ability to control the emission properties of a single type of near-infrared emitting SWNTs over a wide range of wavelengths will enable application of carbon nanotubes in multifunctional photonic devices.

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. Here, we demonstrate strong light-matter coupling in the near infrared using single-walled carbon nanotubes (SWCNTs) in a polymer matrix and a planar metal-clad cavity. By exploiting the exceptional oscillator strength and sharp excitonic transition of (6,5) SWCNTs, we achieve large Rabi splitting (>110 meV), efficient polariton relaxation and narrow band emission (<15 meV). Given their high charge carrier mobility and excellent photostability, SWCNTs represent a promising new avenue towards practical exciton-polariton devices operating at telecommunication 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. The interaction strength is easily tuned by the number of SWCNTs that collectively couple to the plasmonic crystal. Angle- and polarization resolved reflectivity and photoluminescence measurements combined with the coupled-oscillator model confirm strong coupling (coupling strength ∼120 meV). The combination of plasmon–exciton polaritons with the exceptional charge transport properties of SWCNTs should enable practical polariton devices at room temperature and at telecommunication wavelengths.

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. Here we combine the outstanding optical and electronic properties of purified, solution-processed semiconducting (6,5) single-walled carbon nanotubes (SWCNTs) in a microcavity-integrated light-emitting field-effect transistor to realize efficient electrical pumping of exciton-polaritons at room temperature with high current densities (>10 kA cm-2) and tunability in the near-infrared (1,060 nm to 1,530 nm). We demonstrate thermalization of SWCNT polaritons, exciton-polariton pumping rates ∼104 times higher than in current organic polariton devices, direct control over the coupling strength (Rabi splitting) via the applied gate voltage, and a tenfold enhancement of polaritonic over excitonic emission. This powerful material-device combination paves the way to carbon-based polariton emitters and possibly lasers.

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. We incorporate a square array of gold nanodisks into the charge transporting and emissive layer of a polymer LEFET in order to tailor directionality and emission efficiency via the Purcell effect and variation of the fractional local density of states in particular. Angle- and polarization-resolved spectra confirm that the enhanced electroluminescence correlates with the dispersion curves of the surface lattice resonances supported by these structures. These LEFETs reach current densities on the order of 10 kA/cm2, which may pave the way toward practical optoelectronic devices with tailored emission patterns and potentially electrically pumped plasmonic lasers.

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. Consideration of metallic nanotubes allows an analysis of the metallic/semiconducting content, and a process of constraining the fit of highly congested spectra of carbon nanotube solid films according to the spectral weights of each (n, m) species in solution is also presented, allowing for more reliable resolution of overlapping peaks into single (n, m) species contributions.

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. Monochiral (6,5) SWNT films as working electrodes exhibit a narrow absorption band at 997 nm (full width at half-maximum of 55–73 nm) with voltage-dependent optical densities between 0.2 and 4.5 and a modulation depth of up to 43 dB. These (6,5) SWNT notch filters can retain more than 95% of maximum bleaching for several hours under open-circuit conditions. In addition, different levels of transmission can be set by applying constant low voltage (1.5 V) pulses with modulated width or by a given number of fixed short pulses.

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). Depending on the light-matter composition, the rather long-lived plexcitons (>100 fs) undergo highly directional propagation over 20 μm. Near-field energy distributions calculated with the finite-difference time-domain method fully corroborate our experimental results. The previously demonstrated compatibility of this plexcitonic system with electrical excitation opens the path to the realization of a variety of ultrafast active plasmonic devices, cavity-assisted energy transport and low-power optoelectronic components.

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. Mode splitting of more than 70 meV around the trion energy and emission from the new lower polariton branch corroborate a transition from exciton-polaritons (neutral) to trion-polaritons (charged). The estimated charge-to-mass ratio of these trion-polaritons is 200 times higher than that of electrons or holes in carbon nanotubes, which has exciting implications for the realization of polaritonic charge transport.

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. Large current densities are easily achieved due to the high charge carrier mobilities of carbon nanotubes and will facilitate new electrically driven plasmonic devices.