Adenine, deoxyadenosine and deoxyadenosine 5′-monophosphate studied by femtosecond fluorescence upconversion spectroscopy

Gustavsson, T.; Sharonov, A.; Onidas, D.; Markovitsi, Dimitra

doi:10.1016/s0009-2614(02)00290-7

Cited by 127 publications

(163 citation statements)

References 17 publications

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“…However, the lack of structural information on the coumarin-DNA complex, from X-ray or NMR study, keeps www.elsevier.com/locate/cplett unknown the extent of perturbation on the native local structure of DNA. On the other hand, the naturally occurring bases are not appropriate candidates to interrogate the full dynamics of hydration because of their ultrashort lifetimes in the excited states, as reported here and elsewhere using the direct fluorescence up-conversion method [7][8][9].…”

Section: Introductionmentioning

confidence: 93%

Ultrafast decay and hydration dynamics of DNA bases and mimics

Pal

Peón

Zewail

2002

Chemical Physics Letters

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The ultrafast decay of the excited-state of DNA bases, reported here and elsewhere [Peon & Zewail, Chem. Phys. Lett. 348 (2001) 255], makes very difficult the probing of the full hydration dynamics in DNA. Here we present studies of the natural DNA base mimic, 2-aminopurine (2AP), whose excited-state decay is much longer, in water and, for comparison, in bulk ethanol. Guided by these solvation results, which directly reflect the role of orientational and translational diffusion, we reexamine the ultrafast decay rates for the natural nucleotides and nucleosides. The results are important for the mechanism of energy disposal in DNA. Ó

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Section: Introductionmentioning

confidence: 93%

Ultrafast decay and hydration dynamics of DNA bases and mimics

Pal

Peón

Zewail

2002

Chemical Physics Letters

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“…43,44 When TMP and dAMP are dissolved in bulk water, the n-π* transitions shift to higher energies 45,46 and ultrafast emission corresponding to the allowed π-π* transitions is observed. [47][48][49] It would not be surprising that the specific environment created by the double helix, and in particular the presence of multiple electric charges on the phosphate moieties, affects the relative positions of the nπ* and ππ* states. Our fluorescence data obtained for poly(dA).poly(dT) does not allow us to distinguish between emission from nπ* states or charge transfer states (excimer like).…”

Section: A Qualitative Model For Energy Transfermentioning

confidence: 99%

Excited states and energy transfer among DNA bases in double helices

Markovitsi

Gustavsson

Talbot

2007

Photochem Photobiol Sci

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108

174

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Abstract:The study of excited states and energy transfer in DNA double helices has recently gained new interest connected to the development of computational techniques and that of femtosecond spectroscopy. The present article points out contentious questions regarding the nature of the excited states and the occurrence of energy transfer and shows how they are currently approached. Using as example the polymer poly(dA).poly(dT), composed of about 2000 adenine-thymine pairs, a model is proposed on the basis of time-resolved measurements (fluorescence decays, fluorescence anisotropy decays and fluorescence spectra, obtained with femtosecond resolution), associated to steady-state spectra. According to this qualitative model, excitation at 267 nm populates excited states that are delocalized over a few bases (excitons). Ultrafast internal conversion directs the excited state population to the lower part of the exciton band giving rise to fluorescence. Questions needing further investigations, both theoretical and experimental, are underlined with particular emphasis on delicate points related to the complexity and the plasticity of these systems.

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“…[18][19][20] The excited-state lifetimes have been reported recently using many different techniques. [21][22][23][24][25][26][27][28][29][30][31][32][33][34][35][36][37][38][39] These studies report lifetimes on the order of femtoseconds and suggest that nonradiative relaxation proceeds on an ultrafast time scale to the ground state, with the extra energy being transformed into heat.…”

Section: Introductionmentioning

confidence: 99%

Three-State Conical Intersections in Nucleic Acid Bases

2005

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The involvement of three-state conical intersections in the photophysics and radiationless decay processes of the nucleobases has been investigated using multireference configuration interaction methods. Three-state conical intersections have been located for the pyrimidine base, uracil, and the purine base, adenine. In uracil, a three-state degeneracy between the S 0 , S 1 , and S 2 states has been located at 6.2 eV above the ground-state minimum energy. This energy is 0.4 eV higher than vertical excitation to S 2 and at least 1.3 eV higher than the two-state conical intersections found previously. In adenine, two different three-state degeneracies between the S 1 , S 2 , and S 3 states have been located at energies close to the vertical excitation energies. The energetics of these three-state conical intersections suggest they can play a role in a radiationless decay pathway present in adenine. The existence of two different seams of three-state conical intersections indicates that these features are common and complicate the potential energy surfaces of adenine and possibly many other aromatic molecules.

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Adenine, deoxyadenosine and deoxyadenosine 5′-monophosphate studied by femtosecond fluorescence upconversion spectroscopy

Cited by 127 publications

References 17 publications

Ultrafast decay and hydration dynamics of DNA bases and mimics

Ultrafast decay and hydration dynamics of DNA bases and mimics

Excited states and energy transfer among DNA bases in double helices

Three-State Conical Intersections in Nucleic Acid Bases

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