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Optoelectronic properties of single-walled carbon nanotubes and their aggregates.

机译:单壁碳纳米管及其聚集体的光电性能。

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摘要

Precise determination of (n,m) abundance and their optical spectroscopy characteristics of single wall carbon nanotubes (SWNTs) is of pivotal importance for their future involvement in high-end electronic and optoelectronic devices as well as in biosensory applications.; We first developed a methodology to correlate photoluminescence (PL) (n,m)-intensities with (n,m)-SWNT abundance using two dimensional fluorescence spectroscopy of non-covalently functionalized SWNTs sample. Using the extremely sharp diameter-distributed Co-MCM-41 SWNT sample, in conjunction with spectral reconstruction of its near infrared ES11 absorption spectrum, we have been able to independently assess the accuracy of two current theories. Moreover, the reconstruction of the ES11 absorption spectrum provides additional insights of (n,m)-absorption linewidths and the existence of zigzag (n,0) nanotubes.; We also established a methodology to reconstruct the radial breathing modes (RBM) of SWNTs. Using the difference between experimental and E ii(n,m) values of isolated SWNTs. A quantitative assessment was obtained that can be attributed to bundling and possibly excitonic effects. Furthermore, the relative electron-phonon interaction matrix elements (Mph) for 28 (n,m) semiconducting SWNTs species were extracted from the resonance Raman cross sections of individually dispersed HiPco SWNTs. The observed Mph pattern was fitted according to nanotube family (i.e. (2n +m)=constant) and modality ( i.e. mod(n-m,3)=1 or 2) using an empirical equation based on trigonal warping effects. Moreover, the corresponding absolute values of the electron-phonon interaction matrix element were also obtained in both individually dispersed and aggregated states, by utilizing the correlation between RBM overtone and RBM fundamental intensity ratio as a function of laser energy. These values were further used to obtain the Huang-Rhys factor and absolute Mph values for these nanotube species.; Recently, we observed a new class of intermediate frequency modes (IFMs) associated with the ES22 and ES11 optical transitions of bundled HiPco SWNTs. "Step-like" dispersive behavior was observed for these IFMs, along with associated clusters of RBM overtones at higher frequencies. The observed IFM maxima were found to obey a resonance behavior based on a combination of the ES22 and E S11 transition energies, scaled by the inverse diameter of the respective nanotube. Moreover, we found the RBM overtone and IFM Raman intensities are very sensitive to the aggregation state. These observations significantly extended the capability of resonant Raman spectroscopy.
机译:准确确定单壁碳纳米管(SWNT)的(n,m)丰度及其光谱特征对于它们将来涉足高端电子和光电设备以及生物传感应用至关重要。我们首先开发了一种使用非共价功能化SWNTs样品的二维荧光光谱技术将光致发光(PL)(n,m)强度与(n,m)-SWNT丰度相关联的方法。使用直径分布非常尖锐的Co-MCM-41 SWNT样品,结合其近红外ES11吸收光谱的光谱重建,我们已经能够独立评估两种当前理论的准确性。此外,ES11吸收光谱的重建提供了(n,m)吸收线宽和之字形(n,0)纳米管的存在的更多见解。我们还建立了一种方法来重建单壁碳纳米管的radial呼吸模式(RBM)。使用隔离的SWNT的实验值与E ii(n,m)值之差。获得了定量评估,该评估可以归因于束缚和可能的激子效应。此外,从单独分散的HiPco SWNT的共振拉曼截面中提取了28种(n,m)半导体SWNT的相对电子-声子相互作用矩阵元素(Mph)。使用基于三角翘曲效应的经验方程,根据纳米管族(即(2n + m)=恒定)和模态(即mod(n-m,3)= 1或2)拟合观察到的Mph图案。此外,通过利用RBM泛音和RBM基本强度比之间的关系作为激光能量的函数,还可以在单​​独的分散状态和聚集状态下获得电子-声子相互作用矩阵元素的相应绝对值。这些值进一步用于获得这些纳米管种类的Huang-Rhys因子和绝对Mph值。最近,我们观察到与捆绑的HiPco SWNT的ES22和ES11光学跃迁相关的新型中频模式(IFM)。对于这些IFM以及在较高频率下相关的RBM泛音簇,观察到“阶梯状”的分散行为。基于ES22和ES11跃迁能的组合,发现观察到的IFM最大值遵循共振行为,该跃迁能由相应纳米管的反直径定标。此外,我们发现RBM泛音和IFM拉曼强度对聚集状态非常敏感。这些发现大大扩展了共振拉曼光谱的能力。

著录项

  • 作者

    Luo, Zhengtang.;

  • 作者单位

    University of Connecticut.;

  • 授予单位 University of Connecticut.;
  • 学科 Chemistry Polymer.
  • 学位 Ph.D.
  • 年度 2007
  • 页码 148 p.
  • 总页数 148
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 高分子化学(高聚物);
  • 关键词

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