DNA稳定银纳米团簇和载银DNA链之间的动态平衡

IF 4.6 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters Pub Date : 2025-10-09 DOI:10.1021/acs.jpclett.5c02324

Cecilia Cerretani, Donato Ranieri, Giacomo Romolini, Christian Brinch Mollerup, Letizia Liccardo, Elena-Alexandra Niţă, Loredana Latterini, Tom Vosch

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引用次数: 0

摘要

DNA稳定银纳米团簇（DNA- agnc）是一种多用途的发光体，其光物理性质由DNA模板决定。在这项研究中，我们探索了两种nir发射DNA- agnc的不同寻常的温度和浓度依赖行为：一种由两种16碱基DNA低聚物（16mer）稳定，另一种嵌入在这些链的3碱基缩短版本（13mer）中。利用光谱学和质谱的结合，我们发现携带Ag+的DNA链可以可逆地附着在DNA- agnc上，并微调其光物理性质。对于13mer- agnc，我们发现存在三种不同的物种，（13mer）2-[Ag20]10+, (13mer)3-[Ag27]17+和（13mer）4-[Ag34]24+，这取决于浓度和温度。对于由两条16碱基DNA链（16mer）2-[Ag20]10+稳定的AgNC，发射波长和强度随温度变化，尽管没有观察到明显的浓度相关的光谱位移。质谱分析揭示了（16mer）3-[Ag27]17+的存在，时间分辨各向异性揭示了（16mer）2-[Ag20]10+聚集体的形成。这些发现证明了携带Ag+的DNA链和DNA- agnc之间存在动态平衡。

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Dynamic Equilibria between DNA-Stabilized Silver Nanoclusters and Silver-Carrying DNA Strands

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Dynamic Equilibria between DNA-Stabilized Silver Nanoclusters and Silver-Carrying DNA Strands

DNA-stabilized silver nanoclusters (DNA-AgNCs) are versatile emitters whose photophysical properties are defined by the DNA template. In this study, we explore the unusual temperature- and concentration-dependent behavior of two NIR-emissive DNA-AgNCs: one stabilized by two 16-base DNA oligomers (16mer), and another embedded within a 3-base shortened version of these strands (13mer). Using a combination of optical spectroscopy and mass spectrometry, we show that Ag⁺-carrying DNA strands can reversibly attach to DNA-AgNCs and fine-tune their photophysical properties. For 13mer-AgNC, we demonstrate the presence of three different species, (13mer)₂-[Ag₂₀]¹⁰⁺, (13mer)₃-[Ag₂₇]¹⁷⁺, and (13mer)₄-[Ag₃₄]²⁴⁺, depending on concentration and temperature. For the AgNC stabilized by two 16-base DNA strands, (16mer)₂-[Ag₂₀]¹⁰⁺, emission wavelength and intensity vary with temperature, although no significant concentration-dependent spectral shifts are observed. While mass-spectrometry revealed the existence of (16mer)₃-[Ag₂₇]¹⁷⁺, time-resolved anisotropy uncovered the formation of aggregates of (16mer)₂-[Ag₂₀]¹⁰⁺. These findings demonstrate the presence of dynamic equilibria between Ag⁺-carrying DNA strands and DNA-AgNCs.

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来源期刊

The Journal of Physical Chemistry Letters CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY

CiteScore

9.60

自引率

7.00%

发文量

1519

审稿时长

1.6 months

期刊介绍： The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.