Direct measurement of the dynamics of hole hopping in extended DNA G-tracts. an unbiased random walk

Sarah M.Mickley Conron; Arun K. Thazhathveetil; Michael R Wasielewski; Alexander L. Burin; Frederick D Lewis

doi:10.1021/ja106991f

Direct measurement of the dynamics of hole hopping in extended DNA G-tracts. an unbiased random walk

Sarah M.Mickley Conron, Arun K. Thazhathveetil, Michael R Wasielewski, Alexander L. Burin, Frederick D Lewis

Chemistry

Research output: Contribution to journal › Article › peer-review

73 Scopus citations

Abstract

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 A₃G_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 × 10⁹ s ^-1 for a single reversible G-to-G hole hopping step, somewhat faster than the value of 1.2 × 10⁹ s^-1 calculated for A-tract hole hopping. The temperature dependence for hopping in A ₃G₁₃ provides values of E_act = 2.8 kcal/mol and A = 7 × 10⁹ s^-1, consistent with a weakly activated, conformationally gated process.

Original language	English (US)
Pages (from-to)	14388-14390
Number of pages	3
Journal	Journal of the American Chemical Society
Volume	132
Issue number	41
DOIs	https://doi.org/10.1021/ja106991f
State	Published - Oct 20 2010

ASJC Scopus subject areas

Catalysis
Chemistry(all)
Biochemistry
Colloid and Surface Chemistry

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title = "Direct measurement of the dynamics of hole hopping in extended DNA G-tracts. an unbiased random walk",

abstract = "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 A3Gn 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 khop = 4.3 × 109 s -1 for a single reversible G-to-G hole hopping step, somewhat faster than the value of 1.2 × 109 s-1 calculated for A-tract hole hopping. The temperature dependence for hopping in A 3G13 provides values of Eact = 2.8 kcal/mol and A = 7 × 109 s-1, consistent with a weakly activated, conformationally gated process.",

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Direct measurement of the dynamics of hole hopping in extended DNA G-tracts. an unbiased random walk. / Conron, Sarah M.Mickley; Thazhathveetil, Arun K.; Wasielewski, Michael R; Burin, Alexander L.; Lewis, Frederick D.

In: Journal of the American Chemical Society, Vol. 132, No. 41, 20.10.2010, p. 14388-14390.

Research output: Contribution to journal › Article › peer-review

TY - JOUR

T1 - Direct measurement of the dynamics of hole hopping in extended DNA G-tracts. an unbiased random walk

AU - Conron, Sarah M.Mickley

AU - Thazhathveetil, Arun K.

AU - Wasielewski, Michael R

AU - Burin, Alexander L.

AU - Lewis, Frederick D

PY - 2010/10/20

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N2 - 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 A3Gn 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 khop = 4.3 × 109 s -1 for a single reversible G-to-G hole hopping step, somewhat faster than the value of 1.2 × 109 s-1 calculated for A-tract hole hopping. The temperature dependence for hopping in A 3G13 provides values of Eact = 2.8 kcal/mol and A = 7 × 109 s-1, consistent with a weakly activated, conformationally gated process.

AB - 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 A3Gn 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 khop = 4.3 × 109 s -1 for a single reversible G-to-G hole hopping step, somewhat faster than the value of 1.2 × 109 s-1 calculated for A-tract hole hopping. The temperature dependence for hopping in A 3G13 provides values of Eact = 2.8 kcal/mol and A = 7 × 109 s-1, consistent with a weakly activated, conformationally gated process.

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Direct measurement of the dynamics of hole hopping in extended DNA G-tracts. an unbiased random walk

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