School of Electronic Science and Engineering and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing, 210093, China.
Sci Rep. 2017 Sep 11;7(1):11221. doi: 10.1038/s41598-017-11767-z.
Single-wall carbon nanotubes (SWNTs) have been extensively explored as an ultrafast nonlinear optical material. However, due to the numerous electronic and morphological arrangements, a simple and self-contained physical model that can unambiguously account for the rich photocarrier dynamics in SWNTs is still absent. Here, by performing broadband degenerate and non-degenerate pump-probe experiments on SWNTs of different chiralities and morphologies, we reveal strong evidences for the existence of bandgap renormalization in SWNTs. In particularly, it is found that the broadband transient response of SWNTs can be well explained by the combined effects of Pauli blocking and bandgap renormalization, and the distinct dynamics is further influenced by the different sensitivity of degenerate and non-degenerate measurements to these two concurrent effects. Furthermore, we attribute optical-phonon bath thermalization as an underlying mechanism for the observed bandgap renormalization. Our findings provide new guidelines for interpreting the broadband optical response of carbon nanotubes.
单壁碳纳米管 (SWNTs) 已被广泛探索作为超快速非线性光学材料。然而,由于存在众多电子和形态排列,目前仍然缺乏一个简单而完整的物理模型,可以明确解释 SWNTs 中丰富的光载流子动力学。在这里,我们通过对不同手性和形态的 SWNTs 进行宽带简并和非简并泵浦探测实验,揭示了 SWNTs 中带隙重整化存在的有力证据。特别是,我们发现 SWNTs 的宽带瞬态响应可以很好地用 Pauli 阻塞和带隙重整化的综合效应来解释,而不同的简并和非简并测量对这两种并发效应的敏感性差异进一步影响了动力学过程。此外,我们将光声子浴热化归因于观察到的带隙重整化的潜在机制。我们的发现为解释碳纳米管的宽带光响应提供了新的指导。