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Excited-State Dynamics of DNA Duplexes with Different H-Bonding Motifs (41 views)

Zhang Y, De La Harpe K, Beckstead AA, Martínez-fernández L, Improta R, Kohler B

J Phys Chem Lett (ISSN: 1948-7185, 1948-7185electronic), 2016; 7(6): 950-954.

The excited-state dynamics of three distinct forms of the d(GC)9·d(GC)9 DNA duplex were studied by combined time-resolved infrared experiments and quantum mechanical calculations. In the B- and Z-forms, bases on opposite strands form Watson-Crick (WC) base pairs but stack differently because of salt-induced changes in backbone conformation. At low pH, the two strands associate by Hoogsteen (HG) base pairing. Ultraviolet-induced intrastrand electron transfer (ET) triggers interstrand proton transfer (PT) in the B- and Z-forms, but the PT pathway is blocked in the HG duplex. Despite the different decay mechanisms, a common excited-state lifetime of ∼30 ps is observed in all three duplex forms. The ET-PT pathway in the WC duplexes and the solely intrastrand ET pathway in the HG duplex yield the same pair of π-stacked radicals on one strand. Back ET between these radicals is proposed to be the rate-limiting step behind excited-state deactivation in all three duplexes. © 2016 American Chemical Society.

Affiliations ▼
*** IBB - CNR Affiliation

Department of Chemistry and Biochemistry, Montana State University, Bozeman, MT, United States

Department of Physics, United States Air Force Academy, USAF AcademyCO, United States

Consiglio Nationale Delle Ricerche, Istituto di Biostrutture e Bioimmagini, Naples, Italy

Details ▼
Impact factor: 9.353, 5-year impact factor: 8.334

Paper type: Journal Article,

Keywords: Free Radical Reactions, Quantum Theory, Decay Mechanisms, Electron Transfer, Excited State Lifetimes, Excited-State Dynamics, Quantum-Mechanical Calculation, Rate-Limiting Steps, Time-Resolved Infrared, Watson-Crick Base Pairs,

Url: https://www2.scopus.com/inward/record.uri?eid=2-s2.0-84962539733&partnerID=40&md5=891122c1c847208f50bb37e34f2b4a8c

References ▼
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* UV-Induced Proton Transfer between DNA Strands (75 views) (PDF 65 views)
Zhang Y, de La Harpe K, Beckstead AA, Improta R, Kohler B
J Am Chem Soc (ISSN: 0002-7863, 0002-2786, 1520-5126), 2015 Jun 10; 137(22): 7059-7062.
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* Photoinduced Electron Transfer in DNA: Charge Shift Dynamics between 8-Oxo-Guanine Anion and Adenine (83 views)
Zhang Y, Dood J, Beckstead AA, Li X-B, Nguyen KV, Burrows CJ, Improta R, Kohler B
J Phys Chem B (ISSN: 1520-6106, 1520-5207, 1520-5207electronic), 2015; 119(24): 7491-7502.
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2 Records (2 excluding Abstracts and Conferences).
Total impact factor: 16.225 (16.225 excluding Abstracts and Conferences).
Total 5-year impact factor: 15.641 (15.641 excluding Abstracts and Conferences).

Your bibliography query: (([btitle, keywords, abstract] FREE AND [btitle, keywords, abstract] RADICAL AND [btitle, keywords, abstract] REACTIONS AND [btitle, keywords, abstract] QUANTUM AND [btitle, keywords, abstract] THEORY)) AND NOT [id] = 53218

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