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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Excited-State Dynamics of a DNA Duplex in a Deep Eutectic Solvent Probed by Femtosecond Time-Resolved IR Spectroscopy
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Excited-State Dynamics of a DNA Duplex in a Deep Eutectic Solvent Probed by Femtosecond Time-Resolved IR Spectroscopy

机译：由飞秒时间分辨红外光谱探测的深凝胶溶剂中DNA双链体的激发状态动态

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摘要

To better understand how the solvent influences excited-state deactivation in DNA strands, femtosecond time-resolved IR (fs-TRIR) pump–probe measurements were performed on a d(AT)_(9)·d(AT)_(9) duplex dissolved in a deep eutectic solvent (DES) made from choline chloride and ethylene glycol in a 1:2 mol ratio. This solvent, known as ethaline, is a member of a class of ionic liquids capable of solubilizing DNA with minimal disruption to its secondary structure. UV melting analysis reveals that the duplex studied here melts at 18 °C in ethaline compared to 50 °C in aqueous solution. Ethaline has an excellent transparency window that facilitates TRIR measurements in the double-bond stretching region. Transient spectra recorded in deuterated ethaline at room temperature indicate that photoinduced intrastrand charge transfer occurs from A to T, yielding the same exciplex state previously detected in aqueous solution. This state decays via charge recombination with a lifetime of 380 ± 10 ps compared to the 300 ± 10 ps lifetime measured earlier in D_(2)O solution. The TRIR data strongly suggest that the long-lived exciplex forms exclusively in the solvated duplex, and not in the denatured single strands, which appear to have little, if any, base stacking. The longer lifetime of the exciplex state in the DES compared to aqueous solution is suggested to arise from reduced stabilization of the charge transfer state, resulting in slower charge recombination on account of Marcus inverted behavior.
机译：为了更好地了解溶剂如何影响DNA链中的激发状态失活，对广告（AT）_（9）·D（处）进行了飞秒时间分辨的IR（FS-TRIR）泵探针测量测量_（9）双工溶于由氯化胆碱和乙二醇制成的深的共晶溶剂（DES），在1：2摩尔比中。该溶剂，称为含水金属，是一类离子液体的成员，能够溶解DNA，其对其二级结构的严重破坏。 UV熔化分析表明，在这里研究的双链体在乙酸盐中熔化至18℃，而水溶液中的50℃。 Ethaline具有优异的透明度窗口，其有助于双键拉伸区域中的TRIR测量。在室温下记录在氘代乙酸盐中的瞬态光谱表明光诱导的卵形电荷转移从A到T发生，从而产生先前在水溶液中检测到的相同的Exciplex状态。与在D_（2）O溶液中之前测量的300±10 PS寿命相比，该状态通过电荷重组衰减，寿命为380±10 ps。 TRIR数据强烈建议，长寿命的Exciplex在溶化的双层中形成，而不是在变性单链中，这似乎有很少的（如果有的话）。提出了与水溶液相比DES中的Exciplex状态的寿命较长，从降低电荷转移状态的稳定性，导致较慢的电荷重组，因为Marcus倒置行为。

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