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Photoinduced dynamics of guanosine monophosphate in water from broad-band transient absorption spectroscopy and quantum-chemical calculations (50 views)

Karunakaran V, Kleinermanns K, Improta R, Kovalenko SA

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

Abstract
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.

Affiliations ▼
*** IBB - CNR Affiliation

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

Details ▼
Impact factor: 8.58, 5-year impact factor: 8.805

Paper type: Journal Article,

Keywords: 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,

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

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* Singlet excited-state behavior of uracil and thymine in aqueous solution: A combined experimental and computational study of 11 uracil derivatives (95 views)
Gustavsson T, Banyasz A, Lazzarotto E, Markovitsi D, Scalmani G, Frisch MJ, Barone V, Improta R
J Am Chem Soc (ISSN: 0002-7863, 0002-2786, 1520-5126), 2006 Jan 18; 128(2): 607-619.

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1 Records (1 excluding Abstracts and Conferences).
Total impact factor: 7.696 (7.696 excluding Abstracts and Conferences).
Total 5-year impact factor: 11.015 (11.015 excluding Abstracts and Conferences).



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