Reversible surface oxidation and efficient luminescence quenching in semiconductor single-wall carbon nanotubes

Reversible surface oxidation and efficient luminescence quenching in semiconductor single-wall carbon nanotubes
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DOI:
10.1021/ja046526r
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发表时间:
2004-11-24
影响因子:
15
通讯作者:
Brus, LE
Brus, LE
中科院分区:
化学1区
文献类型:
--
作者:
Dukovic, G;White, BE;Brus, LE

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通过对氧化诱导的吸收漂白和低pH下发光猝灭的定量分析,研究了单壁碳纳米管的可逆氧化。这些数据与DFT结构计算相结合,表明纳米管氧化物是1,4-内过氧物。在低pH值下,内过氧物质子化产生过氧化氢碳正离子,在SWNT价带中引入一个空穴。纳米管的发光对空穴掺杂猝灭非常敏感,而吸收相对较强。
We have investigated reversible single-wall carbon nanotube (SWNT) oxidation by quantitative analysis of the oxide-induced absorption bleaching and luminescence quenching at low pH. These data, in combination with DFT structure calculations, suggest that the nanotube oxide is a 1,4-endoperoxide. At low pH, the endoperoxide protonates to create a hydroperoxide carbocation, introducing a hole in the SWNT valence band. Nanotube luminescence is extremely sensitive to quenching by hole-doping, while the absorption is relatively robust.