Coarse-Grained Theory of Biological Charge Transfer with Spatially and Temporally Correlated Noise.
Journal Article (Journal Article)
System-environment interactions are essential in determining charge-transfer (CT) rates and mechanisms. We developed a computationally accessible method, suitable to simulate CT in flexible molecules (i.e., DNA) with hundreds of sites, where the system-environment interactions are explicitly treated with numerical noise modeling of time-dependent site energies and couplings. The properties of the noise are tunable, providing us a flexible tool to investigate the detailed effects of correlated thermal fluctuations on CT mechanisms. The noise is parametrizable by molecular simulation and quantum calculation results of specific molecular systems, giving us better molecular resolution in simulating the system-environment interactions than sampling fluctuations from generic spectral density functions. The spatially correlated thermal fluctuations among different sites are naturally built-in in our method but are not readily incorporated using approximate spectral densities. Our method has quantitative accuracy in systems with small redox potential differences (
Full Text
Duke Authors
Cited Authors
- Liu, C; Beratan, DN; Zhang, P
Published Date
- April 2016
Published In
Volume / Issue
- 120 / 15
Start / End Page
- 3624 - 3633
PubMed ID
- 27008541
Electronic International Standard Serial Number (EISSN)
- 1520-5207
International Standard Serial Number (ISSN)
- 1520-6106
Digital Object Identifier (DOI)
- 10.1021/acs.jpcb.6b01018
Language
- eng