Rationally designed photonic complexes promoting the efficient collection and harnessing of excitation energy are key to artificial photosynthesis and optoelectronics. The precise control over the geometric arrangement and energy flow of photonic materials is in great demand. Mimicking natural light-harvesting systems in terms of multi-pigment complexes well organized by protein scaffolds, herein, we report programmable photonic materials directed by structural DNA templates. Four-helix-bundle DNA origami was used to guide the assembly of the cyanine dye K21 to form closely packed dye aggregates exhibiting strong excitonic coupling between chromophores. This enables sub-micron-scale exciton migration, demonstrated by spectroscopic measurements and theoretical modeling. The DNA-templated dye aggregates acting as “excitonic wires” could mediate directional energy transfer over a half-micrometer distance and were further programmed to achieve geometric complexity and modular bottom-up fabrication of higher order photonic architectures. This work offers a rich toolbox to design and create complex photonic devices and excitonic networks.

合理设计的光子复合物促进激发能量的有效收集和利用是人工光合作用和光电子学的关键。对光子材料的几何排列和能量流的精确控制是非常需要的。在本文中，我们报告了由结构 DNA 模板引导的可编程光子材料，根据由蛋白质支架良好组织的多色素复合物来模拟自然光捕获系统。四螺旋束 DNA 折纸用于指导花青染料 K21 的组装，以形成紧密堆积的染料聚集体，在发色团之间表现出强烈的激子耦合。这使得亚微米级激子迁移成为可能，光谱测量和理论建模证明了这一点。充当“激子线”的 DNA 模板染料聚集体可以在半微米距离上介导定向能量转移，并进一步编程以实现高阶光子架构的几何复杂性和模块化自下而上制造。这项工作为设计和创建复杂的光子器件和激子网络提供了丰富的工具箱。