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Excited-State Dynamics of DNA Duplexes with Different H-Bonding Motifs (55 visite)

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.

Tipo di articolo: Journal Article,

Impact factor: 9.353

Impact factor a 5 anni: 8.334

Parole chiave: 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

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.
*** IBB - CNR ***

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
Zhang, Y., De La Harpe, K., Beckstead, A.A., Improta, R., Kohler, B., UV-Induced Proton Transfer between DNA Strands (2015) J. Am. Chem. Soc., 137, pp. 7059-706

Doorley, G.W., Wojdyla, M., Watson, G.W., Towrie, M., Parker, A.W., Kelly, J.M., Quinn, S.J., Tracking DNA Excited States by Picosecond-Time-Resolved Infrared Spectroscopy: Signature Band for a Charge-Transfer Excited State in Stacked Adenine-Thymine Systems (2013) J. Phys. Chem. Lett., 4, pp. 2739-2744

Stuhldreier, M.C., Temps, F., Ultrafast Photo-Initiated Molecular Quantum Dynamics in the DNA Dinucleotide d(ApG) Revealed by Broadband Transient Absorption Spectroscopy (2013) Faraday Discuss., 163, pp. 173-188

Bucher, D.B., Pilles, B.M., Carell, T., Zinth, W., Charge Separation and Charge Delocalization Identified in Long-Living States of Photoexcited DNA (2014) Proc. Natl. Acad. Sci. U. S. A., 111, pp. 4369-4374

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Zhang, Y., Dood, J., Beckstead, A.A., Li, X.B., Nguyen, K.V., Burrows, C.J., Improta, R., Kohler, B., Efficient UV-Induced Charge Separation and Recombination in an 8-Oxoguanine-Containing Dinucleotide (2014) Proc. Natl. Acad. Sci. U. S. A., 111, pp. 11612-11617

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De La Harpe, K., Crespo-Hernández, C.E., Kohler, B., The Excited-State Lifetimes in a G·C DNA Duplex Are Nearly Independent of Helix Conformation and Base-Pairing Motif (2009) ChemPhysChem, 10, pp. 1421-1425

Doorley, G.W., McGovern, D.A., George, M.W., Towrie, M., Parker, A.W., Kelly, J.M., Quinn, S.J., Picosecond Transient Infrared Study of the Ultrafast Deactivation Processes of Electronically Excited B-DNA and Z-DNA Forms of [poly(dG-dC)]2 (2009) Angew. Chem., Int. Ed., 48, pp. 123-127

Schreier, W.J., Schrader, T.E., Koller, F.O., Gilch, P., Crespo-Hernández, C.E., Swaminathan, V.N., Carell, T., Kohler, B., Thymine Dimerization in DNA is an Ultrafast Photoreaction (2007) Science, 315, pp. 625-629

Zhang, Y., Chen, J., Kohler, B., Hydrogen Bond Donors Accelerate Vibrational Cooling of Hot Purine Derivatives in Heavy Water (2013) J. Phys. Chem. A, 117, pp. 6771-6780

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Huix-Rotllant, M., Brazard, J., Improta, R., Burghardt, I., Markovitsi, D., Stabilization of Mixed Frenkel-Charge Transfer Excitons Extended Across Both Strands of Guanine-Cytosine DNA Duplexes (2015) J. Phys. Chem. Lett., 6, pp. 2247-2251

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Bucher, D.B., Schlueter, A., Carell, T., Zinth, W., Watson-Crick Base Pairing Controls Excited-State Decay in Natural DNA (2014) Angew. Chem., Int. Ed., 53, pp. 11366-11369

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* Photoinduced Electron Transfer in DNA: Charge Shift Dynamics between 8-Oxo-Guanine Anion and Adenine (95 visite)
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* Understanding Electron Transfer across Negatively-Charged Aib Oligopeptides (140 visite)
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* Electron transfer to and conformational preferences of Aib oligo-peptides (70 visite)
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5 Records (5 escludendo Abstract e Conferenze).
Impact factor totale: 14.784 (14.784 escludendo Abstract e Conferenze).
Impact factor a 5 anni totale: 13.555 (13.555 escludendo Abstract e Conferenze).

Interrogazione bibliografica effettuata: (([btitle] "Free Radical Reactions" OR [btitle] "Quantum Theory" OR [btitle] "Decay Mechanisms" OR [btitle] "Electron Transfer" OR [btitle] "Excited State Lifetimes") AND NOT [id] = 53218)

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