The dynamics of excitons in individual semiconducting single-walled carbon nanotubes was studied using time-resolved photoluminescence (PL) spectroscopy. The PL decay from tubes of the same n; m type was found to be monoexponential, however, with lifetimes varying between less than 20 and 200 ps from tube to tube. Competition of nonradiative decay of excitons is facilitated by a thermally activated process, most likely a transition to a low-lying optically inactive trap state that is promoted by a lowfrequency phonon mode.
Individual single-wall carbon nanotubes (SWNTs) and double-wall carbon nanotubes (DWNTs) were suspended in water for optical studies using sodium-cholate and other surfactants. We used time-resolved photoluminescence (PL) spectroscopy to study the influence of tube chirality and diameter as well as of the environment on nonradiative decay in small diameter tubes. The studies provide evidence for PL from small diameter core tubes in DWNTs and for a correlation of nonradiative decay with tube diameter and exciton red shift as induced by interaction with the environment.
We discuss how tight-binding band-structure calculations with a chirality-and diameter-dependent nearest-neighbor hopping integral may be used to relate well resolved features in the UV-VIS-NIR spectra of individual single-wall carbon nanotubes (SWNTs) to electronic excitations in specific tube types. The assignment of (n,m) indices to interband transitions in specific tube types can support a quantitative analysis of absorption spectra which may eventually be used for rapid screening and optimization of sample composition during SWNT synthesis.
We have studied the electronic structure and charge-carrier dynamics of individual single-wall carbon nanotubes (SWNTs) and nanotube ropes using optical and electron-spectroscopic techniques. The electronic structure of semiconducting SWNTs in the band-gap region is analyzed using near-infrared absorption spectroscopy. A semi-empirical expression for E S 11 transition energies, based on tight-binding calculations is found to give striking agreement with experimental data. Time-resolved PL from dispersed SWNT-micelles shows a decay with a time constant of about 15 ps. Using time-resolved photoemission we also find that the electron-phonon (e-ph) coupling in metallic tubes is characterized by a very small e-ph mass-enhancement of 0.0004. Ultrafast electronelectron scattering of photo-excited carriers in nanotube ropes is finally found to lead to internal thermalization of the electronic system within about 200 fs.
Preliminary data suggest that early- and late-fluorescence ratio imaging after ICG administration can be used to distinguish malignant from benign breast lesions.
Using scanning time-domain instrumentation we recorded fluorescence projection mammograms on few breast cancer patients prior, during and after infusion of indocyanine green (ICG), while monitoring arterial ICG concentration by transcutaneous pulse densitometry. Late-fluorescence mammograms recorded after ICG had been largely cleared from the blood by the liver, showed invasive carcinomas at high contrast over a rather homogeneous background, whereas benign lesions did not produce (focused) fluorescence contrast. During infusion, tissue concentration contrast and hence fluorescence contrast is determined by intravascular contributions, whereas late-fluorescence mammograms are dominated by contributions from protein-bound ICG extravasated into the interstitium, reflecting relative microvascular permeabilities of carcinomas and normal breast tissue. We simulated intravascular and extravascular contributions to ICG tissue concentration contrast within a two-compartment unidirectional pharmacokinetic model.
We report on the dynamics of the dielectric function of single-wall carbon nanotubes in the 10-30 THz frequency range after ultrafast laser excitation. The absence of a distinct free-carrier response is attributed to the photogeneration of strongly bound excitons in the tubes with large energy gaps. We find a feature of enhanced transmission caused by the blocking of optical transitions in small-gap tubes. The rapid decay of a featureless background with pronounced dichroism is associated with the increased absorption of spatially localized charge carriers before thermalization is completed.
We present a highly efficient microfluidic fluorescence lifetime-activated droplet sorting (FLADS) approach as a novel technology for droplet manipulation in lab-on-a-chip devices.
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