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π-electron theory of transverse optical excitons in semiconducting single-walled carbon nanotubes

机译:半导体单壁碳纳米管中横向光学激子的π电子理论

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摘要

We present a quantitative theory of optical absorption polarized transverse to the tube axes in semiconducting single-walled carbon nanotubes. Within one-electron theory, transverse optical absorption occurs at an energy that is exactly in the middle of the two lowest longitudinal absorption energies. For nonzero Coulomb interactions between the π electrons, transverse optical absorption is to an exciton state that is strongly blueshifted relative to the longitudinal excitons. Very similar behavior is observed in the π-conjugated polymer polyparaphenylenevinylene, where the optical absorption polarized predominantly perpendicular to the polymer chain axis is blueshifted relative to the absorptions polarized predominantly along the chain axis. The binding energy of the transverse exciton in the nanotubes is considerably smaller than those of the longitudinal excitons. Electron-electron interactions also reduce the relative oscillator strength of the transverse optical absorption. Our theoretical results are in excellent agreement with recent experimental measurements in four chiral nanotubes.
机译:我们提出了一种在半导体单壁碳纳米管中垂直于管轴极化的光吸收的定量理论。在单电子理论中,横向光吸收发生在恰好位于两个最低纵向吸收能量中间的能量处。对于π电子之间的非零库仑相互作用,横向光吸收为相对于纵向激子强烈蓝移的激子状态。在π共轭聚合物聚对亚苯基亚乙烯基中观察到非常相似的行为,其中主要垂直于聚合物链轴偏振的光吸收相对于主要沿着链轴偏振的吸收发生蓝移。纳米管中的横向激子的结合能比纵向激子的结合能小得多。电子-电子相互作用还降低了横向光吸收的相对振荡器强度。我们的理论结果与四个手性纳米管的最新实验测量结果非常吻合。

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