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@article{1124229,
author = {Šponer, Jiří and Mládek, Arnošt and Špačková, Naděžda and Cang, Xiaohui H. and Cheatham, Thomas E. and Grimme, Stefan},
article_location = {WASHINGTON},
article_number = {26},
doi = {http://dx.doi.org/10.1021/ja402525c},
keywords = {DENSITY-FUNCTIONAL THEORY; MOLECULAR-DYNAMICS SIMULATIONS; SUGAR-PHOSPHATE BACKBONE; APPROXIMATE COULOMB POTENTIALS; HUMAN TELOMERIC QUADRUPLEXES; ZETA VALENCE QUALITY; AUXILIARY BASIS-SETS; AMBER FORCE-FIELD; NUCLEIC-ACIDS; CRYSTAL-STRUCTURE},
language = {eng},
issn = {0002-7863},
journal = {Journal of the American Chemical Society},
title = {Relative Stability of Different DNA Guanine Quadruplex Stem Topologies Derived Using Large-Scale Quantum-Chemical Computations},
url = {http://pubs.acs.org/doi/abs/10.1021/ja402525c},
volume = {135},
year = {2013}
}
TY - JOUR
ID - 1124229
AU - Šponer, Jiří - Mládek, Arnošt - Špačková, Naděžda - Cang, Xiaohui H. - Cheatham, Thomas E. - Grimme, Stefan
PY - 2013
TI - Relative Stability of Different DNA Guanine Quadruplex Stem Topologies Derived Using Large-Scale Quantum-Chemical Computations
JF - Journal of the American Chemical Society
VL - 135
IS - 26
SP - 9785-9796
EP - 9785-9796
PB - American Chemical Society
SN - 00027863
KW - DENSITY-FUNCTIONAL THEORY
KW - MOLECULAR-DYNAMICS SIMULATIONS
KW - SUGAR-PHOSPHATE BACKBONE
KW - APPROXIMATE COULOMB POTENTIALS
KW - HUMAN TELOMERIC QUADRUPLEXES
KW - ZETA VALENCE QUALITY
KW - AUXILIARY BASIS-SETS
KW - AMBER FORCE-FIELD
KW - NUCLEIC-ACIDS
KW - CRYSTAL-STRUCTURE
UR - http://pubs.acs.org/doi/abs/10.1021/ja402525c
L2 - http://pubs.acs.org/doi/abs/10.1021/ja402525c
N2 - We provide theoretical predictions of the intrinsic stability of different arrangements of guanine quadruplex (G-DNA) stems. Most computational studies of nucleic acids have applied Molecular Mechanics (MM) approaches using simple pairwise-additive force fields. The principle limitation of such calculations is the highly approximate nature of the force fields. In this study, we for the first time apply accurate QM computations (DFT-D3 with large atomic orbital basis sets) to essentially complete DNA building blocks, seven different folds of the cation stabilized two quartet G-DNA stem, each having more than 250 atoms. The solvent effects are approximated by COSMO continuum solvent We reveal sizable differences between MM and QM descriptions of relative energies of different G-DNA stems, which apparently reflect approximations of the DNA force field. Using the QM energy data, we propose correction to earlier free energy estimates of relative stabilities of different parallel, hybrid, and antiparallel G-stem folds based on classical simulations. The new energy ranking visibly improves the agreement between theory and experiment We predict the 5'-anti-anti-3' GpG dinucleotide step to be the most stable one, closely followed by the 5'-syn-anti-3' step. The results are in good agreement with known experimental structures of 2-, 3-, and 4-quartet G-DNA stems. Besides providing specific results for G-DNA, our study highlights basic limitations of force field modeling of nucleic acids. Although QM computations have their own limitations, mainly the lack of conformational sampling and the approximate description of the solvent, they can substantially improve the quality of calculations currently relying exclusively on force fields.
ER -
ŠPONER, Jiří, Arnošt MLÁDEK, Naděžda ŠPAČKOVÁ, Xiaohui H. CANG, Thomas E. CHEATHAM and Stefan GRIMME. Relative Stability of Different DNA Guanine Quadruplex Stem Topologies Derived Using Large-Scale Quantum-Chemical Computations. \textit{Journal of the American Chemical Society}. WASHINGTON: American Chemical Society, 2013, vol.~135, No~26, p.~9785-9796. ISSN~0002-7863. Available from: https://dx.doi.org/10.1021/ja402525c.
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