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Structural Heterogeneity in Polynucleotide-Facilitated Assembly of Phenothiazine Dyes
The Journal of Physical Chemistry B ( IF 2.8 ) Pub Date : 2018-02-26 00:00:00 , DOI: 10.1021/acs.jpcb.7b12835 Eimer M. Tuite 1 , Bengt Nordén 2
The Journal of Physical Chemistry B ( IF 2.8 ) Pub Date : 2018-02-26 00:00:00 , DOI: 10.1021/acs.jpcb.7b12835 Eimer M. Tuite 1 , Bengt Nordén 2
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The assembly of stacked dyes on DNA is of interest for electron transfer, light harvesting, sensing, and catalysis applications. A combination of UV/vis absorption, linear dichroism (LD), and circular dichroism (CD) was applied to characterize thoroughly the aggregation with DNA of the phenothiazine dyes methylene blue, azure B, and thionine. Aggregates of each dye with [poly(dG-dC)]2, [poly(dA-dT)]2, and calf thymus DNA were explored at high dye:DNA binding ratios, where excess dye groove-binds after all intercalation sites are filled. The organization of the aggregates (dimers, trimers, and multimers) with polydeoxynucleotides displays a structural diversity that depends on DNA sequence, extent of methylation of dye exocyclic amine groups, and ionic strength. The dyes typically form right-handed H-aggregates having negative LD, consistent with stepped stacking along the minor groove. However, aggregates in some dye:DNA aggregates show left-handed chirality or positive LD, indicating unusual modes of aggregation such as formation of adventitious dimers between intercalated and minor groove bound dye. In terms of sequence-dependence, methylene blue shows more extensive aggregation with [poly(dA-dT)]2, while thionine aggregates more with [poly(dG-dC)]2. Azure B has distinctive behavior that is unlike either other dyes. Thus, although these phenothiazine dyes possess a common tricyclic framework, the organization of their polynucleotide-facilitated aggregates depends sensitively on the extent of methylation of the exocyclic amines.
中文翻译：
吩噻嗪染料多核苷酸促进组装中的结构异质性。
DNA上堆叠染料的组装对于电子转移，光收集，传感和催化应用非常重要。结合使用UV / vis吸收，线性二向色性（LD）和圆形二向色性（CD）来彻底表征吩噻嗪染料亚甲基蓝，天蓝色B和硫氨酸与DNA的聚集。每种染料与[poly（dG-dC）] 2和[poly（dA-dT）] 2的聚集体，和小牛胸腺DNA以高的染料：DNA结合比例进行研究，其中所有的插入位点都被填充后，多余的染料沟结合。具有聚脱氧核苷酸的聚集体（二聚体，三聚体和多聚体）的组织显示出结构多样性，取决于DNA序列，染料外环胺基的甲基化程度和离子强度。染料通常会形成具有负LD的右旋H聚集体，这与沿着小凹槽的阶梯式堆积是一致的。但是，某些染料中的聚集体：DNA聚集体显示出左手性或正LD，表明异常的聚集方式，例如在插层的和较小的沟纹结合的染料之间形成了不定的二聚体。就序列依赖性而言，亚甲基蓝显示与[poly（dA-dT）] 2的更广泛聚集，而硫氨酸与[poly（dG-dC）] 2的聚集更多。天青B具有不同于其他任何染料的独特行为。因此，尽管这些吩噻嗪染料具有共同的三环骨架，但是其多核苷酸促进的聚集体的组织敏感地取决于环外胺的甲基化程度。
更新日期：2018-02-26
中文翻译：
吩噻嗪染料多核苷酸促进组装中的结构异质性。
DNA上堆叠染料的组装对于电子转移，光收集，传感和催化应用非常重要。结合使用UV / vis吸收，线性二向色性（LD）和圆形二向色性（CD）来彻底表征吩噻嗪染料亚甲基蓝，天蓝色B和硫氨酸与DNA的聚集。每种染料与[poly（dG-dC）] 2和[poly（dA-dT）] 2的聚集体，和小牛胸腺DNA以高的染料：DNA结合比例进行研究，其中所有的插入位点都被填充后，多余的染料沟结合。具有聚脱氧核苷酸的聚集体（二聚体，三聚体和多聚体）的组织显示出结构多样性，取决于DNA序列，染料外环胺基的甲基化程度和离子强度。染料通常会形成具有负LD的右旋H聚集体，这与沿着小凹槽的阶梯式堆积是一致的。但是，某些染料中的聚集体：DNA聚集体显示出左手性或正LD，表明异常的聚集方式，例如在插层的和较小的沟纹结合的染料之间形成了不定的二聚体。就序列依赖性而言，亚甲基蓝显示与[poly（dA-dT）] 2的更广泛聚集，而硫氨酸与[poly（dG-dC）] 2的聚集更多。天青B具有不同于其他任何染料的独特行为。因此，尽管这些吩噻嗪染料具有共同的三环骨架，但是其多核苷酸促进的聚集体的组织敏感地取决于环外胺的甲基化程度。
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