DNA Origami Chromophore Scaffold Exploiting HomoFRET Energy Transport to Create Molecular Photonic Wires
DNA Origami Chromophore Scaffold Exploiting HomoFRET Energy Transport to Create Molecular Photonic Wires
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DOI：
10.1021/acsanm.0c00038
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发表时间：
2020-04-24
影响因子：
5.9
通讯作者：
Diaz, Sebastian A.
中科院分区：
文献类型：
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作者：
Klein, William P.;Rolczynski, Brian S.;Diaz, Sebastian A.
展示预先排列的供体 - 受体生色团对并参与扩展的福斯特共振能量转移（FRET）级联的DNA支架分子光子线（MPWs）是一种新兴的纳米级光子材料，在数据存储、加密和通信方面有众多潜在应用。为了应用于这些领域，这些器件首先必须在长距离上表现出高效的性能。在此，我们报道了在一个支持14个染料位点系统的6 - 螺旋DNA折纸结构中对FRET的优化，该系统包含一个中心的10个染料的同质FRET（HomoFRET）中继跨度，总长度超过29纳米。通过控制所有可单独寻址位点上染料的存在与否来改变染料密度，呈现出一个极大的优化空间（1024种HomoFRET和16384种总排列）。高通量实验对500多个平行组装的DNA模板进行了测量，从而能够研究HomoFRET转移随荧光团密度和排列的变化。通过稳态光谱实验最初获得的溶液相MPWs内的转移效率仅达到 - 1%。广泛的光物理特性研究，利用六种不同的光谱技术和11种总方法，确定了每个单独组分步骤的FRET效率降低是溶液中转移受限的主要原因。蒙特卡罗和机器学习方法为设计优化提供了更多见解。根据先前的研究结果选择的一组具有代表性的MPW随后在薄膜沉积以及低温条件下进行了表征。在这些改进的条件下，所选的MPWs在29纳米的长度上表现出59±6%的能量传输效率；这比先前报道的优化的DNA MPWs的长度长约25%，效率高10倍。
DNA-scaffolded molecular photonic wires (MPWs) displaying prearranged donor-acceptor chromophore pairs that engage in extended Forster resonance energy transfer (FRET) cascades represent an emerging nanoscale photonic material with numerous potential applications in data storage, encryption, and communications. For translation to such applications, these devices must first demonstrate robust performance with high transfer efficiencies over extended distances. Here, we report the optimization of FRET in a 6-helix DNA origami architecture supporting a 14-dye site system that contains a central 10-dye homogeneous FRET (HomoFRET) relay span and overall extends over 29 nm in length. Varying the dye density by controlling their presence or absence across all of the individually addressable sites presented an incredibly large optimization space (1024 HomoFRET and 16 384 total permutations). High-throughput experiments, with over 500 measurements of DNA templates assembled in parallel, allowed for the study of HomoFRET transfer as a function of fluorophore density and arrangement. Transfer within solution-phase MPWs initially obtained with steady-state spectroscopy experiments revealed values only reaching -1% efficiency. Extensive photophysical characterization, utilizing six different spectroscopic techniques and 11 total methodologies, determined that the diminished FRET efficiency of each individual component step is the principal cause of the limited transfer in solution. Monte Carlo and machine-learning methods provided additional insights into design optimization. A representative MPW set selected based on the previous findings was subsequently characterized in film deposition and also under cryogenic conditions. Under these improved conditions, selected MPWs demonstrated 59 +/- 6% energy transport efficiency over a length of 29 nm; this is similar to 25% longer and 10-fold more efficient than the previously reported optimized DNA MPWs.