Optoelectronics with Carbon Nanotubes

Optoelectronics with Carbon Nanotubes Optoelectronics with Carbon Nanotubes

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(a) Figure III-15. EL spectra with a polarizer aligned along (a) and normal to (b) the tube direction. Symbols are experimental data and solid lines are linear combinations of Lorentz function and the blackbody spectrum, as in Figure III-10. (Inset) Integrated intensity of Lorentz peaks (without background) as a function of power. The fits are exponential functions. As we have already seen in Figure III-13, there is evidence for the E12 (or combination of E12 and E21) transition in some of our EL spectra when both E11 and E22 are observed. Since the E12 state couples more strongly to the perpendicular field and the E11 and E22 states to the parallel field, one should be able to observe the difference in relative intensities of these three peaks if the polarization is changed. We examined under polarizer the device used for Figure III-13, where there was a very weak emission peak about half way between E11 and E22 in the unpolarized measurement. The results are shown in Figure III-16 (a) and (b), with just the E12 peak extracted and normalized in panels (c) and (d). The E12 transition is clearly more prominent in the perpendicular polarization, though it is also seen very weakly in the parallel direction. Also, the overall intensity is weaker than that of E11 or E22, as the depolarization effect of the perpendicularly polarized light causes the weak overall coupling between the E12 excitons and the light emission. A large blue shift in the position of E12 in optical absorption is expected theoretically 19, 133 , which has been observed in PLE experiments. Miyauchi et al. found a smaller exciton 63 (b)

inding energy for perpendicular excitation than for parallel excitation, which is responsible for the blue shift 139 . On the contrary, in our data, no blue shift is observed in the E12 transition (Figure III-16 (b)). A theoretical work by Uryu et al. predicts a large blue shift of the E12 peak that depends on the strength of the Coulomb interaction in SWNTs 133 ; their results show that in the absence of a strong Coulomb interaction, E12 is close to (E11 + E22)/2. In the PL measurements in which large blue shifts were observed in transverse polarization, the tubes were suspended structurally or kept in a surfactant suspension in order to reduce interaction with the environment. In contrast, our devices are directly on the substrate, which significantly increases the dielectric constant of the environment that screens the Coulomb interaction. In our analysis, ε = 3.3 is used which includes ε = 3.9 of the silicon oxide substrate. This significantly reduces the Coulomb interaction in the CNTs on substrate, which could account for the absence of a blue shift of the E12 transition. Lastly, E12 and E21 transitions are degenerate in the single-particle framework, but this no longer applies if the asymmetry between valence and conduction bands are taken into account 140 . Miyauchi et al. has found about a 100 meV difference between the two peaks in perpendicular excitations 30 . However, as has been discussed, all excitonic peaks are significantly broadened and we are not able to determine whether what we consider the E12 transition is actually a double peak consisting of E12 and E21 signatures. 64

(a)<br />

Figure III-15. EL spectra <strong>with</strong> a polarizer aligned along (a) and normal to (b) the tube<br />

direction. Symbols are experimental data and solid lines are linear combinations of<br />

Lorentz function and the blackbody spectrum, as in Figure III-10. (Inset) Integrated<br />

intensity of Lorentz peaks (<strong>with</strong>out background) as a function of power. The fits are<br />

exponential functions.<br />

As we have already seen in Figure III-13, there is evidence for the E12 (or combination of<br />

E12 and E21) transition in some of our EL spectra when both E11 and E22 are observed. Since the<br />

E12 state couples more strongly to the perpendicular field and the E11 and E22 states to the parallel<br />

field, one should be able to observe the difference in relative intensities of these three peaks if<br />

the polarization is changed. We examined under polarizer the device used for Figure III-13,<br />

where there was a very weak emission peak about half way between E11 and E22 in the<br />

unpolarized measurement. The results are shown in Figure III-16 (a) and (b), <strong>with</strong> just the E12<br />

peak extracted and normalized in panels (c) and (d). The E12 transition is clearly more prominent<br />

in the perpendicular polarization, though it is also seen very weakly in the parallel direction.<br />

Also, the overall intensity is weaker than that of E11 or E22, as the depolarization effect of the<br />

perpendicularly polarized light causes the weak overall coupling between the E12 excitons and<br />

the light emission.<br />

A large blue shift in the position of E12 in optical absorption is expected theoretically 19,<br />

133 , which has been observed in PLE experiments. Miyauchi et al. found a smaller exciton<br />

63<br />

(b)

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