Lanthanide-Encoded Multi-functional Tetrahedral DNA for Precise Nanodevice Encoding

The encoding of precise nanodevices is undoubtedly an extremely optimal approach for information storage and multiplex detection. Undeniably, precise control over the nanostructure, composition, and morphology of these devices is of paramount importance. However, most of the tags currently used for encoding are limited by insufficient quantity and low resolution, resulting in deficiencies in accuracy, scalability, and exclusivity of the encoded structures. Here, a series of lanthanide-encoded tetrahedral DNA nanodevices are crafted as unique elemental mass spectrometry-encoded tags. These devices combine the multicomponent interference-free detection capability of elemental encoding with the spatially addressable features of DNA nanostructures. After embedding one to four distinct lanthanide tags (LnTs) and arranging them in equal stoichiometric ratios on different DNA tetrahedral frame cantilevers, the lanthanide nanotags transform into dynamic nanoprobes through combination and fine-tuning. The device can function as a 15-component element tag and generate seven signal outputs. It can respond to three different stimuli when targeting multiple objects simultaneously and is then fed into a semiquantitative analysis based on the isotope dilution method. These DNA nanodevices show strong potential for integration with biological circuits, enabling programmable signal release from their three-dimensional architecture, thereby facilitating even more sophisticated biological identification and logical output.