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首页> 外文期刊>Proceedings of the National Academy of Sciences of the United States of America >Charge transport in DNA in solution: The role of polarons
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Charge transport in DNA in solution: The role of polarons

机译：溶液中DNA中的电荷传输：极化子的作用

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Since the discovery a decade ago of rapid photoincluced electron transfer in DNA over a distance > 4 nm, a large number of experiments and theories have been advanced in the attempt to characterize the transfer, mainly of a radical cation or hole. Particularly influential experiments were carried out by Giese [Giese, B. (2000) Acc. Chem. Res. 33, 631-636] on the sequence G(A)(n)GGG, where G is guanine and A is adenine. These experiments were interpreted as showing that for n > 3, after the holes tunnel through the first three As, they hop onto the bridge of As, where they are localized on a single A and travel further by hopping between neighboring As. Recent experiments of Barton and coworkers [Shao, F., O'Neill, M. A. & Barton, J. K. (2004) Proc. Natl. Acad Sci. USA 101, 1791417919] have, however, established that the hole wavefunctions are delocalized. One of the mechanisms based on delocalized hole wavefunctions that had been investigated, both experimentally and theoretically, is transport by polarons. For one type of polaron, the properties are determined by polarization of the surrounding medium (water and ions, in this case). Theory predicts that this type of polaron is delocalized over approximately four bases in DNA. Transport by these polarons could explain the results of Giese et al. [Giese, B., Amaudrut, J., Kohler, A.-K., Spormann, M. & Wessely, S. (2001) Nature 412, 318-320], recent experimental results of O'Neill and Barton [O'Neill, M. A. & Barton, J. K. (2004) J. Am. Chem. Soc. 126, 11471-11483] concerning the size of the region over which the hole is delocalized, and other experimental observations.
机译：自从十年前发现DNA在大于4 nm的距离内迅速进行光激发电子转移以来，为了表征转移主要是自由基阳离子或空穴的转移，已进行了大量的实验和理论。 Giese [Giese，B.（2000）Acc。化学Res。 33（631-636）]上的序列G（A）（n）GGG，其中G是鸟嘌呤，A是腺嘌呤。这些实验被解释为表明，对于n> 3，在空穴穿过前三个As隧穿之后，它们跳到As的桥上，在那里它们位于单个A上，并通过在相邻的As之间跳动而进一步移动。 Barton及其同事的最新实验[Shao，F.，O'Neill，M. A.＆Barton，J. K.（2004）Proc.Natl.Acad.Sci.USA 90：5873-5877。 Natl。科学院然而，美国101，1791417919]已经确定了空穴波函数是离域的。在实验和理论上已经研究过的基于离域空穴波函数的机理之一是极化子的传输。对于一种类型的极化子，其性质取决于周围介质（在这种情况下为水和离子）的极化。理论预测这种类型的极化子在DNA的大约四个碱基上是离域的。这些极化子的传输可以解释Giese等人的结果。 [Giese，B.，Amaudrut，J.，Kohler，A.-K.，Spormann，M.＆Wessely，S.（2001）Nature 412，318-320]，O'Neill和Barton的最新实验结果[O 'Neill，MA＆Barton，JK（2004）J.Am.化学Soc。 [126，11471-11483]涉及孔在其上离域的区域的大小，以及其他实验观察。

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