Coarse-Grained Theory of Biological Charge Transfer with Spatially and Temporally Correlated Noise.

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