期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 132, 期 41, 页码 14388-14390出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja106991f
关键词
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资金
- Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, DOE [DE-FG02-96ER14604, DE-FG02-99ER 14999]
- NSF CRC [0628130]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [0628130] Funding Source: National Science Foundation
We report the measurement of distance- and temperature-dependent rate constants for charge separation in capped hairpins in which a stilbene hole acceptor and hole donor are separated by A(3)G(n) diblock polypurine sequences consisting of 3 adenines and 1-19 guanines. The longer diblock systems obey the simplest model for an unbiased random walk, providing a direct measurement of k(hop) = 4.3 x 10(9) s(-1) for a single reversible G-to-G hole hopping step, somewhat faster than the value of 1.2 x 10(9) s(-1) calculated for A-tract hole hopping. The temperature dependence for hopping in A(3)G(13) provides values of E-act = 2.8 kcal/mol and A = 7 x 10(9) s(-1), consistent with a weakly activated, conformationally gated process.
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