Evidence for Strong Electronic Correlations in the Spectra of Gate-Doped Single-Wall Carbon Nanotubes
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文摘
We have investigated the photophysical properties of electrochemically gate-doped semiconducting single-wall carbon nanotubes (s-SWNTs). A comparison of photoluminescence (PL) and simultaneously recorded absorption spectra reveals that free-carrier densities correlate well with the first sub-band exciton or trion oscillator strengths but not with PL intensities. We thus used a global analysis of the first sub-band exciton absorption for a detailed investigation of gate-doping, here of the (6,5) SWNT valence band. Our data are consistent with a doping-induced valence band shift according to 螖系v = nb, where n is the free-carrier density, 系v is the valence band edge, and b = 0.15 卤 0.05 eV路nm. We also predict such band gap renormalization of one-dimensional gate-doped semiconductors to be accompanied by a stepwise increase of the carrier density by 螖n = (32meffb)/(蟺鈩?2 (meff is effective carrier mass). Moreover, we show that the width of the spectroelectrochemical window of the first sub-band exciton of 1.55 卤 0.05 eV corresponds to the fundamental band gap of the undoped (6,5) SWNTs in our samples and not to the renormalized band gap of the doped system. These observations as well as a previously unidentified absorption band emerging at high doping levels in the Pauli-blocked region of the single-particle Hartree band structure provide clear evidence for strong electronic correlations in the optical spectra of SWNTs.

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