Sebastian Finn L, Kaminski Leon, Bendel Christoph, Yomogida Yohei, Hosokawa Yuuya, Li Han, Lindenthal Sebastian, Flavel Benjamin S, Yanagi Kazuhiro, Zaumseil Jana
Institute for Physical Chemistry, Universität Heidelberg, Heidelberg, Germany.
Institute for Inorganic Chemistry, Universität Heidelberg, Heidelberg, Germany.
Nat Commun. 2025 Jun 2;16(1):5107. doi: 10.1038/s41467-025-60342-y.
Control over the chiroptical properties of low-dimensional semiconductors is a promising route toward next-generation optoelectronics and photonics. With their helical chirality, single-wall carbon nanotubes (SWCNTs) offer a suitable framework for exploring chiral excitonic states. In addition to intrinsic, one-dimensional excitons, the targeted functionalization of SWCNTs with luminescent defects introduces zero-dimensional quantum states that enhance photoluminescence quantum yields and exhibit single-photon emission at room temperature. Here, we demonstrate that these defect states inherit the chirality of the respective SWCNT enantiomer, as evident from near-infrared circular dichroism. This observation is achieved by utilizing photocatalysis for efficient and versatile functionalization of SWCNTs with luminescent oxygen defects. The employed approach, based on anthraquinone derivatives as photocatalysts, is applicable to SWCNTs with different diameters, in aqueous or organic dispersions, with different surfactants, and even enables lateral patterning of defects in SWCNT networks. Low catalyst concentrations and the absence of cytotoxic metals or reactants make this functionalization method highly biocompatible. Introducing luminescent defects with uniform binding configurations in sorted nanotube enantiomers represents a key step toward chirality control of quantum defects in SWCNTs.
控制低维半导体的手性光学性质是通往下一代光电子学和光子学的一条有前景的途径。单壁碳纳米管（SWCNT）具有螺旋手性，为探索手性激子态提供了一个合适的框架。除了本征的一维激子外，用发光缺陷对SWCNT进行靶向功能化会引入零维量子态，从而提高光致发光量子产率，并在室温下表现出单光子发射。在这里，我们证明这些缺陷态继承了各自SWCNT对映体的手性，这从近红外圆二色性中可以明显看出。这一观察结果是通过利用光催化对SWCNT进行高效且通用的发光氧缺陷功能化而实现的。所采用的方法以蒽醌衍生物作为光催化剂，适用于不同直径的SWCNT，可在水性或有机分散体中、使用不同的表面活性剂，甚至能够对SWCNT网络中的缺陷进行横向图案化。低催化剂浓度以及不存在细胞毒性金属或反应物使得这种功能化方法具有高度的生物相容性。在分选的纳米管对映体中引入具有均匀结合构型的发光缺陷是实现SWCNT量子缺陷手性控制的关键一步。
