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Published on: October 26, 2016
Charge migration in DNA: ion-gated transport
R N Barnett1, C L Cleveland, A Joy
1School of Physics, School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, GA 30332, USA.
Electron hole migration in DNA is controlled by hydrated counterions. Modifying DNA counterion bridges reduced hole mobility, confirming theoretical predictions and demonstrating a new method for controlling charge transport.
Area of Science:
- Biophysics
- Quantum Chemistry
- Molecular Biology
Background:
- Electron holes (radical cations) migrate in DNA via quantum transport.
- This transport is influenced by the dynamic motions of hydrated counterions.
Purpose of the Study:
- To investigate the role of counterion dynamics in DNA charge transport.
- To correlate counterion configurations with charge localization and migration.
- To experimentally validate theoretical predictions of reduced charge mobility.
Main Methods:
- Classical molecular dynamics simulations.
- Large-scale first-principles electronic structure calculations.
- Ultraviolet light-induced DNA cleavage experiments.
Main Results:
- Different counterion configurations lead to varied charge localization and spatial distributions.
- Stochastic fluctuations in counterion configurations induce correlated changes in hole distribution and transport.
- DNA with counterion-starved bridges showed reduced damage, indicating decreased hole mobility.
Conclusions:
- Counterion dynamics play a crucial role in gating electron hole migration in DNA.
- Theoretical models accurately predict the impact of counterion modifications on charge transport.
- Experimental results support the theoretical framework, showing reduced hole mobility in modified DNA structures.
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