Stavros Vasilios G, Verlet Jan R R
Department of Chemistry, University of Warwick, Coventry, CV4 7AL, United Kingdom; email:
Department of Chemistry, University of Durham, Durham, DH1 3LE, United Kingdom; email:
Annu Rev Phys Chem. 2016 May 27;67:211-32. doi: 10.1146/annurev-physchem-040215-112428. Epub 2016 Mar 9.
We summarize how gas-phase ultrafast charged-particle spectroscopy has been used to provide an understanding of the photophysics of DNA building blocks. We focus on adenine and discuss how, following UV excitation, specific interactions determine the fates of its excited states. The dynamics can be probed using a systematic bottom-up approach that provides control over these interactions and that allows ever-larger complexes to be studied. Starting from a chromophore in adenine, the excited state decay mechanisms of adenine and chemically substituted or clustered adenine are considered and then extended to adenosine mono-, di-, and trinucleotides. We show that the gas-phase approach can offer exquisite insight into the dynamics observed in aqueous solution, but we also highlight stark differences. An outlook is provided that discusses some of the most promising developments in this bottom-up approach.
我们总结了气相超快带电粒子光谱如何用于理解DNA构建模块的光物理过程。我们聚焦于腺嘌呤，并讨论在紫外激发后，特定相互作用如何决定其激发态的命运。可以使用一种系统的自下而上的方法来探测动力学，这种方法能够控制这些相互作用，并允许研究越来越大的复合物。从腺嘌呤中的发色团开始，我们考虑了腺嘌呤以及化学取代或聚集的腺嘌呤的激发态衰变机制，然后将其扩展到单、二和三磷酸腺苷。我们表明，气相方法能够对在水溶液中观察到的动力学提供精确的见解，但我们也强调了显著的差异。我们给出了一个展望，讨论了这种自下而上方法中一些最有前景的发展。
