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Title: Low energy secondary electron induced damage of condensed nucleotides

Abstract

Radiation damage and stimulated desorption of nucleotides 2'-deoxyadenosine 5'-monophosphate (dAMP), adenosine 5'-monophosphate (rAMP), 2'-deoxycytidine 5'-monophosphate (dCMP), and cytidine 5'-monophosphate (rCMP) deposited on Au have been measured using x-rays as both the probe and source of low energy secondary electrons. The fluence dependent behavior of the O-1s, C-1s, and N-1s photoelectron transitions was analyzed to obtain phosphate, sugar, and nucleobase damage cross sections. Although x-ray induced reactions in nucleotides involve both direct ionization and excitation, the observed bonding changes were likely dominated by the inelastic energy-loss channels associated with secondary electron capture and transient negative ion decay. Growth of the integrated peak area for the O-1s component at 531.3 eV, corresponding to cleavage of the C—O—P phosphodiester bond, yielded effective damage cross sections of about 23 Mb and 32 Mb (1 Mb = 10 –18 cm 2) for AMP and CMP molecules, respectively. The cross sections for sugar damage, as determined from the decay of the C-1s component at 286.4 eV and the glycosidic carbon at 289.0 eV, were slightly lower (about 20 Mb) and statistically similar for the r- and d- forms of the nucleotides. Here, the C-1s component at 287.6 eV, corresponding to carbons in the nucleobase ring, showedmore » a small initial increase and then decayed slowly, yielding a low damage cross section (~5 Mb). Although there is no statistical difference between the sugar forms, changing the nucleobase from adenine to cytidine has a slight effect on the damage cross section, possibly due to differing electron capture and transfer probabilities.« less

Authors:
ORCiD logo [1];  [1];  [2];  [1]; ORCiD logo [1]
  1. Georgia Inst. of Technology, Atlanta, GA (United States)
  2. Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1559940
Alternate Identifier(s):
OSTI ID: 1523698
Grant/Contract Number:  
AC02-06CH11357; FG02-02ER15337
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 150; Journal Issue: 20; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; XPS; electrons; nucleotides; radiation damage

Citation Formats

McKee, A. D., Schaible, M. J., Rosenberg, R. A., Kundu, S., and Orlando, Thomas M. Low energy secondary electron induced damage of condensed nucleotides. United States: N. p., 2019. Web. doi:10.1063/1.5090491.
McKee, A. D., Schaible, M. J., Rosenberg, R. A., Kundu, S., & Orlando, Thomas M. Low energy secondary electron induced damage of condensed nucleotides. United States. doi:10.1063/1.5090491.
McKee, A. D., Schaible, M. J., Rosenberg, R. A., Kundu, S., and Orlando, Thomas M. Tue . "Low energy secondary electron induced damage of condensed nucleotides". United States. doi:10.1063/1.5090491.
@article{osti_1559940,
title = {Low energy secondary electron induced damage of condensed nucleotides},
author = {McKee, A. D. and Schaible, M. J. and Rosenberg, R. A. and Kundu, S. and Orlando, Thomas M.},
abstractNote = {Radiation damage and stimulated desorption of nucleotides 2'-deoxyadenosine 5'-monophosphate (dAMP), adenosine 5'-monophosphate (rAMP), 2'-deoxycytidine 5'-monophosphate (dCMP), and cytidine 5'-monophosphate (rCMP) deposited on Au have been measured using x-rays as both the probe and source of low energy secondary electrons. The fluence dependent behavior of the O-1s, C-1s, and N-1s photoelectron transitions was analyzed to obtain phosphate, sugar, and nucleobase damage cross sections. Although x-ray induced reactions in nucleotides involve both direct ionization and excitation, the observed bonding changes were likely dominated by the inelastic energy-loss channels associated with secondary electron capture and transient negative ion decay. Growth of the integrated peak area for the O-1s component at 531.3 eV, corresponding to cleavage of the C—O—P phosphodiester bond, yielded effective damage cross sections of about 23 Mb and 32 Mb (1 Mb = 10–18 cm2) for AMP and CMP molecules, respectively. The cross sections for sugar damage, as determined from the decay of the C-1s component at 286.4 eV and the glycosidic carbon at 289.0 eV, were slightly lower (about 20 Mb) and statistically similar for the r- and d- forms of the nucleotides. Here, the C-1s component at 287.6 eV, corresponding to carbons in the nucleobase ring, showed a small initial increase and then decayed slowly, yielding a low damage cross section (~5 Mb). Although there is no statistical difference between the sugar forms, changing the nucleobase from adenine to cytidine has a slight effect on the damage cross section, possibly due to differing electron capture and transfer probabilities.},
doi = {10.1063/1.5090491},
journal = {Journal of Chemical Physics},
number = 20,
volume = 150,
place = {United States},
year = {2019},
month = {5}
}

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