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Ultrafast excited-state dynamics of isocytosine

The result's identifiers

  • Result code in IS VaVaI

    <a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F68081707%3A_____%2F16%3A00471961" target="_blank" >RIV/68081707:_____/16:00471961 - isvavai.cz</a>

  • Alternative codes found

    RIV/00216224:14740/16:00091111

  • Result on the web

    <a href="http://dx.doi.org/10.1039/c6cp01391k" target="_blank" >http://dx.doi.org/10.1039/c6cp01391k</a>

  • DOI - Digital Object Identifier

    <a href="http://dx.doi.org/10.1039/c6cp01391k" target="_blank" >10.1039/c6cp01391k</a>

Alternative languages

  • Result language

    angličtina

  • Original language name

    Ultrafast excited-state dynamics of isocytosine

  • Original language description

    The alternative nucleobase isocytosine has long been considered as a plausible component of hypothetical primordial informational polymers. To examine this hypothesis we investigated the excited-state dynamics of the two most abundant forms of isocytosine in the gas phase (keto and enol). Our surface-hopping nonadiabatic molecular dynamics simulations employing the algebraic diagrammatic construction to the second order [ADC(2)] method for the electronic structure calculations suggest that both tautomers undergo efficient radiationless deactivation to the electronic ground state with time constants which amount to tau(keto) = 182 fs and tau(enol) = 533 fs. The dominant photorelaxation pathways correspond to ring-puckering (pi pi* surface) and C = O stretching/N-H tilting (n pi* surface) for the enol and keto forms respectively. Based on these findings, we infer that isocytosine is a relatively photostable compound in the gas phase and in these terms resembles biologically relevant nucleobases. The estimated S-1> T-1 intersystem crossing rate constant of 8.02 x 10(10) s(-1) suggests that triplet states might also play an important role in the overall excited-state dynamics of the keto tautomer. The reliability of ADC(2)-based surface-hopping molecular dynamics simulations was tested against multireference quantum-chemical calculations and the potential limitations of the employed ADC(2) approach are briefly discussed.

  • Czech name

  • Czech description

Classification

  • Type

    J<sub>x</sub> - Unclassified - Peer-reviewed scientific article (Jimp, Jsc and Jost)

  • CEP classification

    BO - Biophysics

  • OECD FORD branch

Result continuities

  • Project

    Result was created during the realization of more than one project. More information in the Projects tab.

  • Continuities

    I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Others

  • Publication year

    2016

  • Confidentiality

    S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Data specific for result type

  • Name of the periodical

    Physical Chemistry Chemical Physics

  • ISSN

    1463-9076

  • e-ISSN

  • Volume of the periodical

    18

  • Issue of the periodical within the volume

    30

  • Country of publishing house

    GB - UNITED KINGDOM

  • Number of pages

    11

  • Pages from-to

    20208-20218

  • UT code for WoS article

    000381428600022

  • EID of the result in the Scopus database