Atomic defect color centers in solid-state systems hold immense potential to advance various quantum technologies. However, the fabrication of high-quality, densely packed defects presents a significant challenge. Herein we introduce a DNA-programmable photochemical approach for creating organic color-center quantum defects on semiconducting single-walled carbon nanotubes (SWCNTs). Key to this precision defect chemistry is the strategic substitution of thymine with halogenated uracil in DNA strands that are orderly wrapped around the nanotube. Photochemical activation of the reactive uracil initiates the formation of sp³ defects along the nanotube as deep exciton traps, with a pronounced photoluminescence shift from the nanotube band gap emission (by 191 meV for (6,5)-SWCNTs). Furthermore, by altering the DNA spacers, we achieve systematic control over the defect placements along the nanotube. This method, bridging advanced molecular chemistry with quantum materials science, marks a crucial step in crafting quantum defects for critical applications in quantum information science, imaging, and sensing.

中文翻译：

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用卤化 DNA 沿碳纳米管编程 sp3 量子缺陷

固态系统中的原子缺陷色心具有推进各种量子技术的巨大潜力。然而，高质量、密集缺陷的制造提出了重大挑战。在此，我们介绍了一种 DNA 可编程光化学方法，用于在半导体单壁碳纳米管 (SWCNT) 上创建有机色心量子缺陷。这种精确缺陷化学的关键是用卤化尿嘧啶战略性地取代有序缠绕在纳米管周围的 DNA 链中的胸腺嘧啶。反应性尿嘧啶的光化学活化引发了沿纳米管形成 sp ³缺陷作为深激子陷阱，并且光致发光与纳米管带隙发射发生明显的偏移（(6,5)-SWCNT 的光致发光偏移为 191 meV）。此外，通过改变 DNA 间隔区，我们实现了对沿纳米管的缺陷放置的系统控制。这种方法将先进分子化学与量子材料科学联系起来，标志着在量子信息科学、成像和传感等关键应用中制造量子缺陷的关键一步。