用于体积3D打印的三重态融合上转换纳米胶囊
Triplet Fusion Upconversion Nanocapsules for Volumetric 3D Printing
摘要：
双光子光聚合技术无需支撑结构即可实现打印，并最大限度地减少各种材料中的分层伪影。这种体积印刷方法在树脂桶的整个体积中扫描聚焦光源，并利用双光子吸收的二次幂依赖性来仅在焦点处产生光聚合。虽然这种方法具有优势，但由于需要昂贵的超快激光器和极慢的打印速度，双光子光聚合的广泛采用受到阻碍。在这里，我们提出了一个类似的二次过程，三重态-三重态-湮灭驱动的3D打印，其能够在由<4毫瓦功率的连续波激发驱动的焦点处进行体积打印。为了在缸内深处诱导光聚合，关键的进展是将光子上转换溶液纳米封装在用增溶聚合物配体装饰的二氧化硅壳内。这种可扩展的自组装方法允许无散射纳米胶囊分散在各种有机介质中，而不会泄漏胶囊内容物。我们进一步引入激子策略来系统地控制上转换阈值，以支持单体素或并行打印方案，以比基于双光子的3D打印所需的功率密度低多个数量级的功率密度打印。将上转换纳米电容器应用于体积3D打印提供了对体积打印的益处的访问，而没有当前的成本、功率和速度缺点。这里展示的材料为其他三重态聚变上转换控制应用提供了机会。
英文摘要：
Two-photon photopolymerization delivers prints without support structures and minimizes layering artifacts in a broad range of materials. This volumetric printing approach scans a focused light source throughout the entire volume of a resin vat and takes advantage of the quadratic power dependence of two photon absorption to produce photopolymerization exclusively at the focal point. While this approach has advantages, the widespread adoption of two photon photopolymerization is hindered by the need for expensive ultrafast lasers and extremely slow print speeds. Here we present an analogous quadratic process, triplet-triplet-annihilation-driven 3D printing, that enables volumetric printing at a focal point driven by <4 milliwatt-power continuous wave excitation. To induce photopolymerization deep within a vat, the key advance is the nanoencapsulation of photon upconversion solution within a silica shell decorated with solubilizing polymer ligands. This scalable self-assembly approach allows for scatter-free nanocapsule dispersal in a variety of organic media without leaking the capsule contents. We further introduce an excitonic strategy to systematically control the upconversion threshold to support either monovoxel or parallelized printing schemes, printing at power densities multiple orders of magnitude lower than power densities required for two-photon-based 3D printing. The application of upconversion nanocapsules to volumetric 3D printing provides access to the benefits of volumetric printing without the current cost, power, and speed drawbacks. The materials demonstrated here open opportunities for other triplet fusion upconversion-controlled applications.
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