Modeling the Ultrafast Electron Attachment Dynamics of Solvated Uracil

Anstöter, Cate S.; DelloStritto, Mark; Klein, Michael L.; Matsika, Spiridoula

doi:10.1021/acs.jpca.1c05288

Modeling the Ultrafast Electron Attachment Dynamics of Solvated Uracil

Journal Article · Wed Aug 04 00:00:00 EDT 2021 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI:https://doi.org/10.1021/acs.jpca.1c05288· OSTI ID:1999113

^[1]; ^[2]; Klein, Michael L. ^[2]; ^[2]

Temple University, Philadelphia, PA (United States); Princeton University, Department of Chemistry
Temple University, Philadelphia, PA (United States)

Electron attachment to DNA by low energy electrons can lead to DNA damage, so a fundamental understanding of how electrons interact with the components of nucleic acids in solution is an open challenge. In solution, low energy electrons can generate presolvated electrons, e_pre^–, which are efficiently scavanged by pyrimidine nucleobases to form transient negative ions, able to relax to either stable valence bound anions or undergo dissociative electron detachment or transfer to other parts of DNA/RNA leading to strand breakages. In order to understand the initial electron attachment dynamics, this paper presents a joint molecular dynamics and high-level electronic structure study into the behavior of the electronic states of the solvated uracil anion. Both the valence π* and nonvalence e_pre^– states of the solvated uracil system are studied, and the effect of the solvent environment and the geometric structure of the uracil core are uncoupled to gain insight into the physical origin of the stabilization of the solvated uracil anion. As a result, solvent reorganization is found to play a dominant role followed by relaxation of the uracil core.

View Accepted Manuscript (DOE)

Research Organization:: Princeton University, NJ (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-05CH11231; SC0019394

OSTI ID:: 1999113

Alternate ID(s):: OSTI ID: 1853197

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Journal Name: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory Journal Issue: 32 Vol. 125; ISSN 1089-5639

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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