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Mapping the ultrafast dynamics of adenine onto its nucleotide and oligonucleotides by time-resolved photoelectron imaging.

机译：通过时间分辨光电子成像将腺嘌呤的超快动力学映射到其核苷酸和寡核苷酸上。

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The intrinsic photophysics of nucleobases and nucleotides following UV absorption presents a key reductionist step toward understanding the complex photodamage mechanisms occurring in DNA. The decay mechanism of adenine in particular has been the focus of intense investigation, as has how these correlate to those of its more biologically relevant nucleotide and oligonucleotides in aqueous solution. Here, we report on time-resolved photoelectron imaging of the deprotonated 3′-deoxy-adenosine-5′-monophosphate nucleotide and the adenosine di- and trinucleotides. Through a comparison of gas- and solution-phase experiments and available theoretical studies, the dynamics of the base are shown to be relatively insensitive to the surrounding environment. The decay mechanism primarily involves internal conversion from the initially populated 1ππ* states to the ground state. The relaxation dynamics of the adenosine oligonucleotides are similar to those of the nucleobase, in contrast to the aqueous oligonucleotides, where a fraction of the ensemble forms long-lived excimer states.
机译：紫外线吸收后，核碱基和核苷酸的固有光物理性质为理解DNA中复杂的光损伤机理提供了关键的还原论步骤。特别是腺嘌呤的衰变机制一直是研究的重点，这些机制如何与其在水溶液中与生物学上更相关的核苷酸和寡核苷酸相关。在这里，我们报告去质子化的3'-脱氧腺苷-5'-单磷酸核苷酸和腺苷二核苷酸和三核苷酸的时间分辨光电子成像。通过气相和溶液相实验的比较以及可用的理论研究，表明该基础的动力学对周围环境相对不敏感。衰减机制主要涉及从最初填充的1ππ*状态到基态的内部转换。与水性寡核苷酸相反，腺苷寡核苷酸的松弛动力学类似于核碱基的松弛动力学，在水性寡核苷酸中，一部分集合形成长寿命的准分子态。

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