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High-Energy Long-Lived Mixed Frenkel-Charge-Transfer Excitons: From Double Stranded (AT)n to Natural DNA (95 visite)

Vayá I, Brazard J, Huix-rotllant M, Thazhathveetil AK, Lewis FD, Gustavsson T, Burghardt I, Improta R, Markovitsi D

Chemistry (ISSN: 0947-6539, 1521-3765, 1521-3765electronic), 2016; 22(14): 4904-4914.

Tipo di articolo: Journal Article, , Impact factor: 5.317, Impact factor a 5 anni: 5.184, Url: https://www2.scopus.com/inward/record.uri?eid=2-s2.0-84961730181&partnerID=40&md5=22e242fce4f2130ecd20c2a49167a4f6

Parole chiave: Dna, Excitons, Fluorescence Spectroscopy, Hypochromism, Quantum Chemistry,

Affiliazioni: *** IBB - CNR ***
LIDYL, CEA, CNRS, Université Paris Saclay, Gif-sur-Yvette, France
Institut für Physikalische und Theoretische Chemie, Goethe-Universität, Max-von-Laue-Str. 7, Frankfurt am Main, Germany
Department of Chemistry, Northwestern University, Evanston, IL, United States
Istituto Biostrutture e Bioimmagini-Consiglio, Nazionale Delle Ricerche, Via mezzocannone 16, Napoli, Italy


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The electronic excited states populated upon absorption of UV photons by DNA are extensively studied in relation to the UV-induced damage to the genetic code. Here, we report a new unexpected relaxation pathway in adenine-thymine double-stranded structures (AT)n. Fluorescence measurements on (AT)n hairpins (six and ten base pairs) and duplexes (20 and 2000 base pairs) reveal the existence of an emission band peaking at approximately 320 nm and decaying on the nanosecond time scale. Time-dependent (TD)-DFT calculations, performed for two base pairs and exploring various relaxation pathways, allow the assignment of this emission band to excited states resulting from mixing between Frenkel excitons and adenine-to-thymine charge-transfer states. Emission from such high-energy long-lived mixed (HELM) states is in agreement with their fluorescence anisotropy (0.03), which is lower than that expected for π-π∗ states (≥0.1). An increase in the size of the system quenches π-π∗ fluorescence while enhancing HELM fluorescence. The latter process varies linearly with the hypochromism of the absorption spectra, both depending on the coupling between π-π∗ and charge-transfer states. Subsequently, we identify the common features between the HELM states of (AT)n structures with those reported previously for alternating (GC)n: High emission energy, low fluorescence anisotropy, nanosecond lifetimes, and sensitivity to conformational disorder. These features are also detected for calf thymus DNA in which HELM states could evolve toward reactive π-π∗ states, giving rise to delayed fluorescence. High-energy long-lived mixed (HELM) excitons are populated during excited-state relaxation in (AT)n duplexes. They result from mixing between Frenkel excitons and adenine-to-thymine charge-transfer states and extend over at least four bases on both strands. The properties of HELM states (high emission energy, low fluorescence anisotropy, nanosecond lifetime, and sensitivity to conformational disorder) are also detected for natural DNA. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Nessun risultato.
UV-Induced Proton Transfer between DNA Strands (accesso riservato) (108 visite)

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Staiano M, Saviano M, Herman P, Grycznyski Z, Fini C, Varriale A, Parracino A, Kold AB, Rossi M, D'Auria S
* Time-resolved fluorescence spectroscopy and molecular dynamics simulations point out the effects of pressure on the stability and dynamics of the porcine odorant-binding protein (143 visite)
Biopolymers (ISSN: 0006-3525, 0006-6352, 0006-3525print), 2008; 89(4): 284-291.
Impact Factor: 2.823
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Salvatore A, Cigliano L, Bucci EM, Corpillo D, Velasco S, Carlucci A, Pedone C, Abrescia P
* Haptoglobin binding to apolipoprotein A-I prevents damage from hydroxyl radicals on its stimulatory activity of the enzyme lecithin-cholesterol acyl-transferase (112 visite)
Biochemistry (ISSN: 0006-2960, 1520-4995, 1520-4995electronic), 2007 Oct 2; 46(39): 11158-11168.
Impact Factor: 3.368
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Ragno R, Simeoni S, Castellano S, Vicidomini C, Mai A, Caroli A, Tramontano A, Bonaccini C, Trojer P, Bauer I, Brosch G, Sbardella G
* Small molecule inhibitors of histone arginine methyltransferases: Homology modeling, molecular docking, binding mode analysis, and biological evaluations (137 visite)
J Med Chem (ISSN: 0022-2623, 1520-4804, 0022-2623print), 2007 Mar 22; 50(6): 1241-1253.
Impact Factor: 4.895
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Mai A, Rotili D, Tarantino D, Ornaghi P, Tosi F, Vicidomini C, Sbardella G, Nebbioso A, Miceli M, Altucci L, Filetici P
* Small-molecule inhibitors of histone acetyltransferase activity: Identification and biological properties (115 visite)
J Med Chem (ISSN: 0022-2623, 1520-4804, 0022-2623print), 2006 Nov 16; 49(23): 6897-6907.
Impact Factor: 5.115
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Barone V, Newton MD, Improta R
* Dissociative electron transfer in donor - Peptide - Acceptor systems: Results for kinetic parameters from a density functional/polarizable continuum model (81 visite)
J Phys Chem B (ISSN: 1520-6106, 1520-5207, 1520-5207electronic), 2006 Jun 29; 110(25): 12632-12639.
Impact Factor: 4.115
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Improta R, Barone V, Newton MD
* A Parameter Free Quantum Mechanical Approach To The Calculation Of Electron Transfer Rates For Large Systems In Solution (81 visite)
Chemphyschem (ISSN: 1439-4235, 1439-7641, 1439-7641electronic), 2006 Jun 12; 7(6): 1211-1215.
Impact Factor: 3.449
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Cittadini A, Monti MG, Iaccarino G, Di Rella F, Tsichlis PN, Di Gianni A, Strömer H, Sorriento D, Peschle C, Trimarco B, Saccà L, Condorelli G
* Adenoviral gene transfer of Akt enhances myocardial contractility and intracellular calcium handling (118 visite)
Gene Ther Gene Therapy (ISSN: 0969-7128), 2006; 13(1): 8-19.
Impact Factor: 4.782
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Mai A, Rotili D, Ornaghi P, Tosi F, Vicidomini C, Sardella G, Nebbioso A, Altucci L, Filatici P
* Identification of small molecules inhibitors of GCN5 histone acetyltransferase activity (95 visite)
Arkivoc (ISSN: 1424-6376), 2006; 6(VIII): 24-37.
Impact Factor: 0.8
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Improta R, Antonello S, Formaggio F, Maran F, Rega N, Barone V
* Understanding Electron Transfer across Negatively-Charged Aib Oligopeptides (184 visite)
J Phys Chem B (ISSN: 1520-6106, 1520-5207, 1520-5207electronic), 2005 Jan 20; 109(2): 1023-1033.
Impact Factor: 4.033
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Lauceria R, Purrellob R
* Transfer, memory and amplification of chirality in porphyrin aggregates (77 visite)
Supramol Chem Supramolecular Chemistry (ISSN: 1061-0278), 2005; 17(1-2): 61-66.
Impact Factor: 1.715
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Barone V, Formaggio F, Improta R, Polo F, Maran F
* Electron transfer to and conformational preferences of Aib oligo-peptides (115 visite)
Proc Electrochem Soc, 2004; 10: 29-32.
Impact Factor: 0
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Caliendo G, Fiorino F, Grieco P, Perissutti E, De Luca S, Giuliano A, Santelli G, Califano D, Severino B, Santagada V
Synthesis and biological activity of pseudopeptides inhibitors of Ras farnesyl transferase containing unconventional amino acids (125 visite)
Farmaco (ISSN: 0014-827x), 1999 Nov; 54(11-12): 785-790.
Impact Factor: 0.406
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Caraglia M, Tagliaferri P, Correale P, Genua G, Pinto A, Del Vecchio S, Esposito G, Bianco AR
CYTOSINE-ARABINOSIDE INCREASES THE BINDING OF I-125 LABELED EPIDERMAL GROWTH-FACTOR AND I-125 TRANSFERRIN AND ENHANCES THE IN-VITRO TARGETING OF HUMAN TUMOR-CELLS WITH ANTI-(GROWTH FACTOR-RECEPTOR) MAB (115 visite)
Cancer Immunology Immunotherapy (ISSN: 0340-7004), 1993 Sep; 37(3): 150-156.
Impact Factor: 1.269
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Caraglia M, Correale P, Genua G, Pepe S, Del Vecchio S, Esposito G, Bianco AR, Tagliaferri P
EPIDERMAL GROWTH-FACTOR (EGFR) AND TRANSFERRIN (TRFR) RECEPTOR UP-REGULATION IS INDUCED BY ARABINOSIDE CYTOSINE (ARA-C) ON HUMAN TUMOR-CELLS (95 visite)
(ISSN: 0361-090x), 1993; 17(2): 337-338.
Impact Factor: 0.838
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44 Records (43 escludendo Abstract e Conferenze).
Impact factor totale: 181.722 (178.739 escludendo Abstract e Conferenze).
Impact factor a 5 anni totale: 173.394 (170.022 escludendo Abstract e Conferenze).







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