单壁碳纳米管中发光sp $^{3}$缺陷引起的激子-极化激元布居
Population of Exciton-Polaritons via Luminescent sp$^{3}$ Defects in Single-Walled Carbon Nanotubes
摘要：
半导体单壁碳纳米管（SWCNTs）由于其稳定的激子、窄的近红外发射和高的载流子迁移率而成为一种重要的强光物质耦合材料。此外，它们已经作为量子光源出现，这是由于受控地引入具有能够实现单光子发射的红移跃迁的发光量子缺陷（sp $^{3}$ -缺陷）。单壁碳纳米管复杂的物理学和极化激元凝聚的总体目标提出了激子-极化激元如何填充以及如何优化的问题。可能的弛豫过程的贡献，即，利用角度分辨反射率和时间分辨光致发光测量研究了具有大范围失谐的微腔的声声子散射、振动辅助散射和辐射泵浦。我们发现，平面微腔中单壁碳纳米管激子极化激元的主要布居机制是辐射泵浦。因此，由于纳米管的低光致发光量子产率而导致的极化激元布居的限制可以通过发光sp $^{3}$缺陷来克服。在不改变极化激元分支结构的情况下，通过这些发射缺陷的辐射泵浦导致具有大光子分数的失谐的极化激元群体增加高达10倍。因此，具有sp $^{3}$缺陷的SWCNT的受控和可调谐的官能化呈现了朝向明亮和有效的极化激元器件的可行路线。
英文摘要：
Semiconducting single-walled carbon-nanotubes (SWCNTs) are an interesting material for strong-light matter coupling due to their stable excitons, narrow emission in the near infrared and high charge carrier mobilities. Furthermore, they have emerged as quantum light sources as a result of the controlled introduction of luminescent quantum defects (sp$^{3}$-defects) with red-shifted transitions that enable single-photon emission. The complex photophysics of SWCNTs and overall goal of polariton condensation pose the question of how exciton-polaritons are populated and how it might be optimized. The contributions of possible relaxation processes, i.e., scattering with acoustic phonons, vibrationally assisted scattering, and radiative pumping, are investigated using angle-resolved reflectivity and time-resolved photoluminescence measurements on microcavities with a wide range of detunings. We show that the predominant population mechanism for SWCNT exciton-polaritons in planar microcavities is radiative pumping. Consequently, the limitation of polariton population due to the low photoluminescence quantum yield of nanotubes, can be overcome by luminescent sp$^{3}$ defects. Without changing the polariton branch structure, radiative pumping through these emissive defects leads to an up to 10-fold increase of the polariton population for detunings with a large photon fraction. Thus, the controlled and tunable functionalization of SWCNTs with sp$^{3}$ defects presents a viable route towards bright and efficient polariton devices.
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