UV-induced long-lived decays in solvated pyrimidine nucleosides resolved at the MS-CASPT2/MM level (378 views)
Phys Chem Chem Phys (ISSN: 1463-9084electronic, 1463-9076linking), 2018 Mar 7; 20(10): 6877-6890.
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Paper type: Journal Article,
Impact factor: 3.454, 5-year impact factor: 3.859
Url: https://www.scopus.com/inward/record.uri?eid=2-s2.0-85043491107&doi=10.1039%2fc7cp08235e&partnerID=40&md5=1e03b36a20125667feca621b9f4db20c
Keywords: Not available.
Affiliations:
*** IBB - CNR ***
Dipartimento di Chimica Industriale "Toso Montanari", Universita di Bologna, Viale del Risorgimento 4, I-40136 Bologna, Italy. marco.garavelli@unibo.it.,
Univ Lyon, ENS de Lyon, CNRS, Unversité Lyon 1, Laboratoire de Chimie UMR 5182, Allée d'Italie 46, Lyon, FR-69342, France
Istituto di Biostrutture e Bioimmagini CNR, Via Mezzocannone 16, Napoli, I-80134, Italy
LIDYL, CEA, CNRS, Université Paris-Saclay, Gif-sur-Yvette, F-91191, France
References:
Not available.
Phys Chem Chem Phys (ISSN: 1463-9084electronic, 1463-9076linking), 2018 Mar 7; 20(10): 6877-6890.
Export to BibTeX Export to EndNote
Paper type: Journal Article,
Impact factor: 3.454, 5-year impact factor: 3.859
Url: https://www.scopus.com/inward/record.uri?eid=2-s2.0-85043491107&doi=10.1039%2fc7cp08235e&partnerID=40&md5=1e03b36a20125667feca621b9f4db20c
Keywords: Not available.
Affiliations:
*** IBB - CNR ***
Dipartimento di Chimica Industriale "Toso Montanari", Universita di Bologna, Viale del Risorgimento 4, I-40136 Bologna, Italy. marco.garavelli@unibo.it.,
Univ Lyon, ENS de Lyon, CNRS, Unversité Lyon 1, Laboratoire de Chimie UMR 5182, Allée d'Italie 46, Lyon, FR-69342, France
Istituto di Biostrutture e Bioimmagini CNR, Via Mezzocannone 16, Napoli, I-80134, Italy
LIDYL, CEA, CNRS, Université Paris-Saclay, Gif-sur-Yvette, F-91191, France
References:
Not available.
UV-induced long-lived decays in solvated pyrimidine nucleosides resolved at the MS-CASPT2/MM level
The most relevant 'dark' electronic excited states in DNA/RNA pyrimidine nucleosides are mapped in water employing hybrid MS-CASPT2/MM optimisations with explicit solvation and including the sugar. Conical intersections (CIs) between initially accessed bright 1ππ∗ and the lowest energy dark 1nπ∗ excited states, involving the lone pair localised on the oxygen and/or nitrogen atoms are characterised. They are found in the vicinities of the Franck-Condon (FC) region and are shown to facilitate non-adiabatic population transfer. The excited state population of the 1nOπ∗ state, localised in the carbonyl moiety on all pyrimidine nucleosides, is predicted to rapidly evolve to its minimum, displaying non-negligible potential energy barriers along its non-radiative decay, and accounting for the ps signal registered in pump-probe experiments as well as for an efficient population of the triplet state. Cytidine displays an additional 1nNπ∗ state localised in the N3 atom and that leads to its excited state minimum displaying large potential energy barriers in the pathway connecting to the CI with the ground state. Sugar-to-base hydrogen/proton transfer processes are assessed in solution for the first time, displaying a sizable barrier along its decay and thus being competitive with other slow decay channels in the ps and ns timescales. A unified deactivation scheme for the long-lived channels of pyrimidine nucleosides is delivered, where the 1nOπ∗ state is found to mediate the long-lived decay in the singlet manifold and act as the doorway for triplet population and thus accounting for the recorded phosphorescence and, more generally, for the transient/photoelectron spectral signals registered up to the ns timescale. © the Owner Societies 2018.
The most relevant 'dark' electronic excited states in DNA/RNA pyrimidine nucleosides are mapped in water employing hybrid MS-CASPT2/MM optimisations with explicit solvation and including the sugar. Conical intersections (CIs) between initially accessed bright 1ππ∗ and the lowest energy dark 1nπ∗ excited states, involving the lone pair localised on the oxygen and/or nitrogen atoms are characterised. They are found in the vicinities of the Franck-Condon (FC) region and are shown to facilitate non-adiabatic population transfer. The excited state population of the 1nOπ∗ state, localised in the carbonyl moiety on all pyrimidine nucleosides, is predicted to rapidly evolve to its minimum, displaying non-negligible potential energy barriers along its non-radiative decay, and accounting for the ps signal registered in pump-probe experiments as well as for an efficient population of the triplet state. Cytidine displays an additional 1nNπ∗ state localised in the N3 atom and that leads to its excited state minimum displaying large potential energy barriers in the pathway connecting to the CI with the ground state. Sugar-to-base hydrogen/proton transfer processes are assessed in solution for the first time, displaying a sizable barrier along its decay and thus being competitive with other slow decay channels in the ps and ns timescales. A unified deactivation scheme for the long-lived channels of pyrimidine nucleosides is delivered, where the 1nOπ∗ state is found to mediate the long-lived decay in the singlet manifold and act as the doorway for triplet population and thus accounting for the recorded phosphorescence and, more generally, for the transient/photoelectron spectral signals registered up to the ns timescale. © the Owner Societies 2018.
UV-induced long-lived decays in solvated pyrimidine nucleosides resolved at the MS-CASPT2/MM level
| ▼ Functional characterization of synthetic organic molecules of therapeutic interest |
| ▼ Molecular dynamics simulation approach to study UV-induced DNA damage |
UV-induced long-lived decays in solvated pyrimidine nucleosides resolved at the MS-CASPT2/MM level
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View Export to BibTeX Export to EndNote
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Improta R
* Photophysics and photochemistry of thymine deoxy-dinucleotide in water: A PCM/TD-DFT quantum mechanical study (390 views)
J Phys Chem B (ISSN: 1520-6106, 1520-5207, 1520-5207electronic), 2012 Dec 13; 116(49): 14261-14274.
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View Export to BibTeX Export to EndNote
Dolga AM, Letsche T, Gold M, Doti N, Bacher M, Chiamvimonvat N, Dodel R, Culmsee C
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View Export to BibTeX Export to EndNote
Zannetti A, Iommelli F, Speranza A, Salvatore M, Del Vecchio S
* 3'-deoxy-3'-18F-fluorothymidine (FLT) PET/CT to guide therapy with epidermal growth factor receptor (EGFR) antagonists and Bcl-xL inhibitors in non-small cell lung cancer (716 views)
J Nucl Med (ISSN: 0161-5505, 1535-5667, 1535-5667electronic), 2012 Mar 1; 53(3): 443-450.
Impact Factor: 5.774
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Zannetti A, Iommelli F, Speranza A, Salvatore M, Del Vecchio S
* 3'-deoxy-3'-18F-fluorothymidine PET/CT to guide therapy with epidermal growth factor receptor antagonists and Bcl-xL inhibitors in non-small cell lung cancer (678 views)
J Nucl Med (ISSN: 1535-5667, 0161-5505, 1535-5667electronic), 2012 Mar 1; 53(3): 443-450.
Impact Factor: 5.774
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Roviello GN, Ricci A, Bucci EM, Pedone C
* Synthesis, biological evaluation and supramolecular assembly of novel analogues of peptidyl nucleosides (1680 views)
Mol Biosyst (ISSN: 1742-206x, 1742-2051, 1742-2051electronic), 2011 May; 7(5): 1773-1778.
Impact Factor: 3.534
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Del Vecchio S, Zannetti A, Fonti R, Iommelli F, Pizzuti LM, Lettieri A, Salvatore M
* PET/CT in cancer research: From preclinical to clinical applications (727 views)
Contrast Media Mol Imaging (ISSN: 1555-4309, 1555-4309linking), 2010 Jul; 5(4): 190-200.
Impact Factor: 4.02
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Roviello GN, Benedetti E, Pedone C, Bucci EM
* Nucleobase-containing peptides: An overview of their characteristic features and applications (978 views)
Amino Acids (ISSN: 0939-4451, 1438-2199, 1438-2199electronic), 2010 Jun; 39(1): 45-57.
Impact Factor: 4.106
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Banyasz A, Gustavsson T, Keszei E, Improta R, Markovitsi D
* Effect of amino substitution on the excited state dynamics of uracil (411 views)
Photochem Photobiol Sci (ISSN: 1474-905x), 2008 Jul; 7(7): 765-768.
Impact Factor: 2.144
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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 (352 views)
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 (437 views)
Pharmacol Res Academic Press, 2008 Jun 23; 350(1-3): 1-2.
Impact Factor: 3.976
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Ohlenschlager O, Wohnert J, Bucci E, Seitz S, Hafner S, Ramachandran R, Zell R, Gorlach M
* The Structure of the Stemloop D Subdomain of Coxsackievirus B3 Cloverleaf RNA and Its Interaction with the Proteinase 3C (771 views)
Structure (ISSN: 0969-2126, 1878-4186, 0969-2126linking), 2004; 12(2): 237-248.
Impact Factor: 5.185
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28 Records (28 excluding Abstracts).
Total impact factor: 128.042 (128.042 excluding Abstracts).
Total 5 year impact factor: 113.989 (113.989 excluding Abstracts).
Total impact factor: 128.042 (128.042 excluding Abstracts).
Total 5 year impact factor: 113.989 (113.989 excluding Abstracts).
378 views. Last view on Friday 31 May 2024, 23:41:39
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