Electroluminescence et radiation thermique dans les nanotubes de carbone

We present here a spectroscopic study of the light emission properties of different nanotube devices with the aim to clarify the different mechanisms leading to the light emission.;The first study consists of taking measurements from a thick (∼ 450 nm) macroscopic suspended carbon nanotube film connected between two electrodes. A significant increase of the temperature is expected when voltage is applied since thermal dissipation by the substrate is suppressed for this configuration. In imaging mode, we observed that infrared light is emitted from the entire area of the film instead of being localized. This observation demonstrates that the light emission arise from thermal emission. Spectra measured on this device all present a smooth response, characteristic of that of a blackbody. As expected for a pure thermal source, the results fit well the Planck formula. Because the Planck formula is temperature dependant, it became possible to extract a lower limit of the temperature of the film as a function of voltage. The temperature increases more or less from 350K to 600K when the voltage increases from 0.1V to 1.6V.;The second study is made using a sub-monolayer network of carbon nanotubes interconnected together to form a semiconducting layer. The large number of tube-tube junctions in the networks limits the current and prevents the temperature to rise significantly at higher bias. The intimate contact between the network and the substrate also prevent the temperature of the film to increase significantly due to a good thermalizaton. Hence, electroluminescence from excitonic recombination is expected to be dominant over heat radiation for this type of devices. First, spatial resolution measurements on long channel network devices shows that the light-emitting zone is always located near the minority charge injector contact. This result demonstrates that light emission arises from electroluminescence in network from a bipolar current. Thermal emission can therefore be ruled out as the main mechanism of emission in this case. We also studied network field effect transistor with shorter channel length in order to extract the light emission spectra. As expected, all spectra exhibit a broad peak (linewidth ∼ 200 meV) with a maxima that correspond to the first excitonic level in semiconducting nanotube, the so-called ES11 . These results support bipolar (electron-hole) current recombination as the main mechanism of emission and allowed to rule out the impact excitation mechanism of electroluminescence. We also observed that the spectrum of the emission is red-shifted with respect to the corresponding absorption spectrum. This spectral feature reveals that large diameter carbon nanotubes contribute the most to the electroluminescence spectra. Two different effects are proposed to explain why the emission is dominated by the large diameter nanotubes: (i) the carrier density distribution is higher on large diameter nanotubes and (ii) an effective energy transfer process takes place from small to large diameter nanotubes.;We finally measured light emission spectra from individual carbon nanotube transistors in air and under vacuum. In air, each spectrum is characterized by a peak that is narrower (∼ 80-150 meV) than those measured in network FETs (∼ 200 meV), suggesting that many carbon nanotubes do emit light simultaneously in the network. Moreover, the peak position of individual nanotube FETs changes from device to device, as expected for electroluminescence from individual carbon nanotubes having different diameters. This set of results suggests that the main mechanism of light emission from individual nanotube FETs in air is dominated by electroluminescence. In vacuum, although low current spectra have a peaked-shape similar to the one measured in air, spectra taken at high current present a totally different shape. The general shape is a blackbody tail that is similar to the spectra measured for suspended film. This result strongly suggests that light emission arises from thermal radiation in individual FETs when measured under vacuum and at high bias. An analysis of the spectra revealed however small deviations between the experimental spectra and the best fit to the Planck law. Three explanations are proposed for the deviations: an electroluminescence contribution that is superimposed to the thermal component; additional contribution from the spectral emissivity response of the nanotube; artifacts due to the low resolution of the setup calibration. More experiment will be needed to distinguish between these explanations. (Abstract shortened by UMI.).