% IMPORTANT: The following is UTF-8 encoded. This means that in the presence
% of non-ASCII characters, it will not work with BibTeX 0.99 or older.
% Instead, you should use an up-to-date BibTeX implementation like “bibtex8” or
% “biber”.
@ARTICLE{Zeleny:22673,
author = {Zeleny, T. and Ruckenbauer, M. and Aquino, A.J.A. and
Müller, Th. and Lankas, F. and Drsata, T. and Hase, W.L.
and Nachtigallova, D. and Lischka, H.},
title = {{S}trikingly {D}ifferent {E}ffects of {H}ydrogen {B}onding
on the {P}hotodynamics of {I}ndividual {N}ucleobases in
{DNA}: {C}omparison of {G}uanine and {C}ytosine},
journal = {Journal of the American Chemical Society},
volume = {134},
issn = {0002-7863},
address = {Washington, DC},
publisher = {American Chemical Society},
reportid = {PreJuSER-22673},
pages = {13662 - 13669},
year = {2012},
note = {This work has been supported by the Austrian Science Fund
within the framework of the Special Research Program and F41
Vienna Computational Materials Laboratory (ViCoM). This work
was also performed as part of research supported by the
National Science Foundation Partnership in International
Research and Education (PIRE) Grant No. OISE-730114; support
was provided by the Robert A. Welch Foundation under Grant
No. D-0005. The calculations were performed in part at the
Vienna Scientific Cluster (project nos. 70019 and 70151).
The research at IOCB was part of the project RVO:61388963.
This work was also supported by the grants of the Grant
Agency of the Czech Republic (P208/12/1318 and GACR
203/09/H046), the grant of the Czech Ministry of Education,
Youth and Sport (LH11021) and Operational Program Research
and Development for Innovations - European Regional
Development Fund (project CZ.1.05/2.1.00/03.0058 of the
Ministry of Education, Youth and Sports of the Czech
Republic). F.L. acknowledges the support by the J. E.
Purkyne Fellowship provided by the Academy of Sciences of
the Czech Republic.},
abstract = {Ab initio surface hopping dynamics calculations were
performed to study the photophysical behavior of cytosine
and guanine embedded in DNA using a quantum
mechanical/molecular mechanics (QM/MM) approach. It was
found that the decay rates of photo excited cytosine and
guanine were affected in a completely different way by the
hydrogen bonding to the DNA environment. In case of
cytosine, the geometrical restrictions exerted by the
hydrogen bonds did not influence the relaxation time of
cytosine significantly due to the generally small cytosine
ring puckering required to access the crossing region
between excited and ground state. On the contrary, the
presence of hydrogen bonds significantly altered the
photodynamics of guanine. The analysis of the dynamics
indicates that the major contribution to the lifetime
changes comes from the interstrand hydrogen bonds. These
bonds considerably restricted the out-of-plane motions of
the NH(2) group of guanine which are necessary for the
ultrafast decay to the ground state. As a result, only a
negligible amount of trajectories decayed into the ground
state for guanine embedded in DNA within the simulation time
of 0.5 ps, while for comparison, the isolated guanine
relaxed to the ground state with a lifetime of about 0.22
ps. These examples show that, in addition to phenomena
related to electronic interactions between nucleobases,
there also exist relatively simple mechanisms in DNA by
which the lifetime of a nucleobase is significantly enhanced
as compared to the gas phase.},
keywords = {J (WoSType)},
cin = {JSC},
ddc = {540},
cid = {I:(DE-Juel1)JSC-20090406},
pnm = {Scientific Computing (FUEK411) / 411 - Computational
Science and Mathematical Methods (POF2-411)},
pid = {G:(DE-Juel1)FUEK411 / G:(DE-HGF)POF2-411},
shelfmark = {Chemistry, Multidisciplinary},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:22845192},
UT = {WOS:000307699000025},
doi = {10.1021/ja3028845},
url = {https://juser.fz-juelich.de/record/22673},
}