Revisiting the Hole Size in Double Helical DNA with Localized Orbital Scaling Corrections.
Journal
The journal of physical chemistry. B
ISSN: 1520-5207
Titre abrégé: J Phys Chem B
Pays: United States
ID NLM: 101157530
Informations de publication
Date de publication:
23 04 2020
23 04 2020
Historique:
pubmed:
10
4
2020
medline:
15
5
2021
entrez:
10
4
2020
Statut:
ppublish
Résumé
The extent of electronic wave function delocalization for the charge carrier (electron or hole) in double helical DNA plays an important role in determining the DNA charge transfer mechanism and kinetics. The size of the charge carrier's wave function delocalization is regulated by the solvation induced localization and the quantum delocalization among the π stacked base pairs at any instant of time. Using a newly developed localized orbital scaling correction (LOSC) density functional theory method, we accurately characterized the quantum delocalization of the hole wave function in double helical B-DNA. This approach can be used to diagnose the extent of delocalization in fluctuating DNA structures. Our studies indicate that the hole state tends to delocalize among 4 guanine-cytosine (GC) base pairs and among 3 adenine-thymine (AT) base pairs when these adjacent bases fluctuate into degeneracy. The relatively small delocalization in AT base pairs is caused by the weaker π-π interaction. This extent of delocalization has significant implications for assessing the role of coherent, incoherent, or flickering coherent carrier transport in DNA.
Identifiants
pubmed: 32272019
doi: 10.1021/acs.jpcb.0c03112
pmc: PMC7456463
mid: NIHMS1620525
doi:
Substances chimiques
Guanine
5Z93L87A1R
Cytosine
8J337D1HZY
DNA
9007-49-2
Thymine
QR26YLT7LT
Types de publication
Journal Article
Research Support, N.I.H., Extramural
Research Support, Non-U.S. Gov't
Research Support, U.S. Gov't, Non-P.H.S.
Langues
eng
Sous-ensembles de citation
IM
Pagination
3428-3435Subventions
Organisme : NIGMS NIH HHS
ID : R01 GM048043
Pays : United States
Organisme : NIGMS NIH HHS
ID : R01 GM061870
Pays : United States
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