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Photoinduced dynamics of guanosine monophosphate in water from broad-band transient absorption spectroscopy and quantum-chemical calculations (116 visite)

Karunakaran V, Kleinermanns K, Improta R, Kovalenko SA

J Am Chem Soc (ISSN: 0002-7863, 0002-2786, 1520-5126), 2009; 131(16): 5839-5850.



Tipo di articolo: Journal Article,

Impact factor: 8.58, Impact factor a 5 anni: 8.805

Url: http://www.scopus.com/inward/record.url?eid=2-s2.0-69949158122&partnerID=40&md5=dee8189784a4b05a511f694c031baf0e

Parole chiave: Aqueous Solutions, Biexponential, Biexponential Decay, Broad Bands, Bulk Solvents, Conical Intersection, Femtoseconds, Fluorescence Lifetimes, Guanine Rings, Guanosines, Internal Conversions, Monophosphates, Out-Of-Plane Displacement, Ph Range, Photo-Induced, Photoinduced Dynamics, Protonated, Quantum-Chemical Calculation, Quantum-Mechanical Calculation, Specific Solvation, State-To-State Relaxation, Time-Dependent, Transient Absorption Spectroscopies, Ultra-Fast, Ultrafast Decay, Various Ph, Biomolecules, Excited States, Ground State, Ph Effects, Quantum Chemistry, Water Absorption, Guanosine Phosphate, Article, Light, Proton Transport,

Affiliazioni:

*** IBB - CNR ***
Department of Chemistry, Humboldt University, Brook-Taylor Street-2, D-12489 Berlin, Germany
Department of Physical Chemistry, Heinrich-Heine-University, University Street-1, D-40225 Düsseldorf, Germany
Dipartimento di Chimica, Università Federico II, Complesso Universitario Monte S. Angelo Via Cintia, I-80126 Napoli, Italy
Istituto Biostrutture e Bioimmagini, CNR, Via Mezzocannone 16, I-80134 Napoli, Italy



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Guanosine monophosphate (GMP) in aqueous solutions has been studied with femtosecond broad-band transient absorption spectroscopy and by quantum-mechanical calculations. The sample was excited at 267 or 287 nm and probed between 270 and 1000 nm with 100 fs resolution, for various pH values between 2 and 7. At pH 2, when the guanine ring is ground-state protonated (GMPH +), we observe isosbestic behavior indicating state-to-state relaxation. The relaxation is biexponential, τ 1 = 0.4 ps, τ 2 = 2.2 ps, and followed by slower internal conversion with τ 3 = 167 ps. For nonprotonated GMP in the pH range 7-4, we find biexponential decay in the region 400-900 nm (τ 1 = 0.22 ps, τ 2 = 0.9 ps), whereas, between 270 and 400 nm, the behavior is triexponential with one growing, τ 1 = 0.25 ps, and two decaying, τ 2 = 1.0 ps, τ 3 = 2.5 ps, components. The excited-state evolution is interpreted with the help of quantumchemical calculations, performed at the time-dependent PBE0 level accounting for bulk solvent effects and specific solvation. The computed dynamics involves L a and L b bright excited states, whereas the n 0π and π σ dark excited states play a minor role. Independent of the pH, the photoinduced evolution involves ultrafast L b→ L a conversion (τ ba « 100 fs) and exhibits the presence of a wide planar plateau on L a. For neutral GMP a barrierless path connects this region to a conical intersection (CI) with the ground state, giving an account of the ultrafast decay of this species. For protonated GMPH + the system evolves into a stable minimum L a min characterized by out-of-plane displacement of NH and CH groups, which explains the longer (167 ps) fluorescence lifetime. © 2009 American Chemical Society.
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J Phys Chem B (ISSN: 1520-6106, 1520-5207, 1520-5207electronic), 2008 Sep 4; 112(35): 10769-10772.
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Gustavsson T, Bányász A, Sarkar N, Markovitsi D, Improta R
* Assessing solvent effects on the singlet excited state lifetime of uracil derivatives: A femtosecond fluorescence upconversion study in alcohols and D2O (93 visite)
Chem Phys (ISSN: 0301-0104), 2008 Jun 23; 350(1-3): 186-192.
Impact Factor: 1.961
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Gustavsson T, Banyasz A, Sarkar N, Markovitsi D, Improta R
* Statin: New life for an old drug (128 visite)
Pharmacol Res Academic Press, 2008 Jun 23; 350(1-3): 1-2.
Impact Factor: 3.976
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29 Records (27 escludendo Abstract e Conferenze).
Impact factor totale: 189.655 (185.601 escludendo Abstract e Conferenze).
Impact factor a 5 anni totale: 194.873 (190.763 escludendo Abstract e Conferenze).







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