Long-lived Ag106+ luminescence and a split DNA scaffold
Long-lived Ag106+ luminescence and a split DNA scaffold
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DOI：
10.1063/5.0056214
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发表时间：
2021-06-28
影响因子：
4.4
通讯作者：
Lewis, David
中科院分区：
文献类型：
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作者：
Petty, Jeffrey T.;Carnahan, Savannah;Lewis, David
分子银簇发射可见光到近红外线，并且可以使用DNA链形成特定的发色团。研究了C（4）AC（4）TC（3）G对Ag-10（6+）的选择性配位和包封作用，该生色团具有两个不同的电子跃迁。绿色发射强烈且迅速，phi = 18%，τ = 1.25 ns，近红外发光较弱，τ = 50 μ s时较慢，并且部分被氧猝灭，表明磷光。这种寿命可以通过DNA宿主来调节，并且我们考虑具有相似序列但不同结构的C（4）AC（4）TC（3）G的两种衍生物。在一个变体中，切除胸腺嘧啶以在原本完整的链中产生脱碱基缺口。在另一种方法中，去除共价磷酸键以将DNA支架分成两个片段。相对于连续的链，断裂的模板使发光衰减加快两倍，这种差异可能是由于更大的DNA柔性。这些修改表明，DNA可以在结构上进行调整，以调节其银簇加合物中的亚稳态电子状态。由AIP Publishing独家授权出版。
Molecular silver clusters emit across the visible to near-infrared, and specific chromophores can be formed using DNA strands. We study C(4)AC(4)TC(3)G that selectively coordinates and encapsulates Ag-10(6+), and this chromophore has two distinct electronic transitions. The green emission is strong and prompt with phi = 18% and tau = 1.25 ns, and the near-infrared luminescence is weaker, slower with tau = 50 mu s, and is partly quenched by oxygen, suggesting phosphorescence. This lifetime can be modulated by the DNA host, and we consider two derivatives of C(4)AC(4)TC(3)G with similar sequences but distinct structures. In one variant, thymine was excised to create an abasic gap in an otherwise intact strand. In the other, the covalent phosphate linkage was removed to split the DNA scaffold into two fragments. In relation to the contiguous strands, the broken template speeds the luminescence decay by twofold, and this difference may be due to greater DNA flexibility. These modifications suggest that a DNA can be structurally tuned to modulate metastable electronic states in its silver cluster adducts. Published under an exclusive license by AIP Publishing.