Institute of Physical and Theoretical Chemistry & Department of Chemistry and Pharmacy, University of Würzburg, D-97074 Würzburg, Germany.
ACS Nano. 2010 Dec 28;4(12):7161-8. doi: 10.1021/nn101612b. Epub 2010 Nov 24.
Photoluminescence quantum yields and nonradiative decay of the excitonic S(1) state in length fractionated (6,5) single-wall carbon nanotubes (SWNTs) are studied by continuous wave and time-resolved fluorescence spectroscopy. The experimental data are modeled by diffusion limited contact quenching of excitons at stationary quenching sites including tube ends. A combined analysis of the time-resolved photoluminescence decay and the length dependence of photoluminescence quantum yields (PL QYs) from SWNTs in sodium cholate suspensions allows to determine the exciton diffusion coefficient D = 10.7 ± 0.4 cm(2)s(-1) and lifetime τ(PL) for long tubes of 20 ± 1 ps. PL quantum yields Φ(PL) are found to scale with the inverse diffusion coefficient and the square of the mean quenching site distance, here l(d) = 120 ± 25 nm. The results suggest that low PL QYs of SWNTs are due to the combination of high-diffusive exciton mobility with the presence of only a few quenching sites.
通过连续波和时间分辨荧光光谱研究了长度分级的(6,5)单壁碳纳米管(SWNTs)中激子 S(1)态的光致发光量子产率和非辐射衰减。通过扩散限制的激子在静止猝灭位置(包括管端)处的接触猝灭来对实验数据进行建模。对SWNTs 在胆酸钠悬浮液中的时间分辨光致发光衰减和光致发光量子产率(PLQY)的长度依赖性的综合分析,允许确定激子扩散系数 D = 10.7 ± 0.4 cm(2)s(-1)和长管的寿命 τ(PL)为 20 ± 1 ps。发现 PL 量子产率 Φ(PL)与扩散系数的倒数和平均猝灭位距离的平方成比例,此处 l(d) = 120 ± 25 nm。结果表明,SWNTs 的低 PLQY 是由于高扩散激子迁移率与仅存在少数猝灭位置的组合所致。