Abstract
Characterizing the photophysical properties of nucleic acid bases and base pairs presents a major challenge to theoretical modelling. In this Chapter, we focus on the contributions of nonadiabatic ab initio molecular dynamics (na-AIMD) simulations towards unravelling the dynamical mechanisms governing the radiationless decay of DNA and RNA building blocks. The na-AIMD method employed here is based entirely on plane-wave density functional theory and couples nonadiabatically the Kohn-Sham electronic ground state to the restricted open-shell Kohn-Sham first excited singlet state by means of a surface hopping scheme. This approach has been applied to a variety of different nucleobases and tautomers thereof. Gas phase calculations on canonical tautomers serve as a reference to study both substitution and solvation effects. The na-AIMD simulations of nonradiative decay in aqueous solution allow direct comparison with the gas phase results as the same computational setup can be used in both cases. Solute and solvent are both treated explicitly on an equal footing
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Doltsinis, N.L., Markwick, P.R., Nieber, H., Langer, H. (2008). Ultrafast Radiationless Decay in Nucleic Acids: Insights From Nonadiabatic Ab Initio Molecular Dynamics. In: Shukla, M.K., Leszczynski, J. (eds) Radiation Induced Molecular Phenomena in Nucleic Acids. Challenges and Advances In Computational Chemistry and Physics, vol 5. Springer, Dordrecht. https://doi.org/10.1007/978-1-4020-8184-2_10
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