Structure and Dynamics of Oligonucleotides in the Gas Phase
Structure and Dynamics of Oligonucleotides in the Gas Phase
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DOI：
10.1002/anie.201406910
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发表时间：
2015-01-07
影响因子：
16.6
通讯作者：
Orozco, Modesto
中科院分区：
文献类型：
--
作者：
Arcella, Annalisa;Dreyer, Jens;Orozco, Modesto
通过将离子迁移率质谱实验与亚毫秒经典和从头算分子动力学相结合，我们首次充分表征了电喷雾电离条件下气相中模型核酸的动态系综。所研究的寡核苷酸展开蒸发后，失去记忆的解决方案的结构，并探索真正的气相构象空间。与我们最初的预期相反，寡核苷酸在三个不同的时间尺度（多皮秒，纳秒和亚毫秒）中显示出非常丰富的动力学。较短的时间尺度动力学具有量子力学性质，并导致共价结构的变化，而其他两个是经典的起源。总的来说，这项研究表明，重新评估我们的观点的物理核酸蒸发是必要的。
By combining ion-mobility mass spectrometry experiments with sub-millisecond classical and abinitio molecular dynamics we fully characterized, for the first time, the dynamic ensemble of a model nucleic acid in the gas phase under electrospray ionization conditions. The studied oligonucleotide unfolds upon vaporization, loses memory of the solution structure, and explores true gas-phase conformational space. Contrary to our original expectations, the oligonucleotide shows very rich dynamics in three different timescales (multi-picosecond, nanosecond, and sub-millisecond). The shorter timescale dynamics has a quantum mechanical nature and leads to changes in the covalent structure, whereas the other two are of classical origin. Overall, this study suggests that a re-evaluation on our view of the physics of nucleic acids upon vaporization is needed.