Abstract
We report free energy barriers for the ground-state dissociation of the guanosine nucleotide anion in solution, employing implicit and explicit solvation models. The latter was based on the Free Energy Perturbation technique and Monte Carlo simulations. For the lowest-energy structure, both solvation models indicate a solvent-induced transition from a dipole-bound state in the gas phase to a π ∗ valence state in solution. The free barrier estimates obtained from explicit and implicit solvation are in fair agreement with each other, although significantly overestimated in comparison to a previously reported explicit solvation model based on ab initio molecular dynamics simulations. Accounting for corrections related to the different DFT functionals used in the present and previous studies significantly improves the agreement.
Similar content being viewed by others
References
S. Gohlke, E. Illenberger, Europhys. News 33, 207 (2002)
L. Sanche, Nature 461, 358 (2009)
E. Alizadeh, L. Sanche, Chem. Rev. 112, 5578 (2012)
B. Boudaïffa, P. Cloutier, D. Hunting, M.A. Huels, L. Sanche, Science 287, 1658 (2000)
C. Winstead, V. McKoy, Radiation Physics and Chemistry 77, 1258 (2008)
I. Baccarelli, I. Bald, F.A. Gianturco, E. Illenberger, J. Kopyra, Phys. Rep. 508, 1 (2011)
C.R. Wang, J. Nguyen, Q.B. Lu, J. Am. Chem. Soc. 131, 11320 (2009)
J. Simons, Acc. Chem. Res. 39, 772 (2006)
J. Gu, J. Leszczynski, H.F. Schaefer III, Chem. Rev. 112, 5603 (2012)
J. Tomasi, B. Mennucci, R. Cammi, Chem. Rev. 105, 2999 (2005)
P. Schyman, A. Laaksonen, J. Am. Chem. Soc. 130, 12254 (2008)
M. Smyth, J. Kohanoff, J. Am. Chem. Soc. 134, 9122 (2012)
M.J. Frisch, G.W. Trucks, H.B. Schlegel, G.E. Scuseria, M.A. Robb, J.R. Cheeseman, G. Scalmani, V. Barone, B. Mennucci, G.A. Petersson, H. Nakatsuji, M. Caricato, X. Li, H.P. Hratchian, A.F. Izmaylov, J. Bloino, G. Zheng, J.L. Sonnenberg, M. Hada, M. Ehara, K. Toyota, R. Fukuda, J. Hasegawa, M. Ishida, T. Nakajima, Y. Honda, O. Kitao, H. Nakai, T. Vreven, J.A. Montgomery Jr., J.E. Peralta, F. Ogliaro, M. Bearpark, J.J. Heyd, E. Brothers, K.N. Kudin, V.N. Staroverov, R. Kobayashi, J. Normand, K. Raghavachari, A. Rendell, J.C. Burant, S.S. Iyengar, J. Tomasi, M. Cossi, N. Rega, J.M. Millam, M. Klene, J.E. Knox, J.B. Cross, V. Bakken, C. Adamo, J. Jaramillo, R. Gomperts, R.E. Stratmann, O. Yazyev, A.J. Austin, R. Cammi, C. Pomelli, J.W. Ochterski, R.L. Martin, K. Morokuma, V.G. Zakrzewski, G.A. Voth, P. Salvador, J.J. Dannenberg, S. Dapprich, A.D. Daniels, Ö. Farkas, J.B. Foresman, J.V. Ortiz, J. Cioslowski, D.J. Fox, Gaussian 09 Revision D.01 (Gaussian Inc. Wallingford CT, 2009)
A.D. Becke, J. Chem. Phys. 98, 1372 (1993)
N.A. Richardson, S.S. Wesolowski, H.F. Schaefer III, J. Am. Chem. Soc. 124, 10163 (2002)
C. Peng, B.H. Schlegel, Israel J. Chem. 33, 449 (1993)
C. Peng, P.Y. Ayala, H.B. Schlegel, M.J. Frisch, J. Comput. Chem. 17, 49 (1996)
H.B. Schlegel, Wiley Interdisciplin. Rev.: Comput. Mol. Sci. 1, 790 (2011)
Y. Zhao, D.G. Truhlar, Theor. Chem. Acc. 120, 215 (2008)
A.V. Marenich, C.J. Cramer, D.G. Truhlar, J. Phys. Chem. B 113, 6378 (2009)
B. Mennucci, J. Tomasi, J. Chem. Phys. 106, 5151 (1997)
A.K. Rappe, C.J. Casewit, K.S. Colwell, W.A. Goddard, W.M. Skiff, J. Am. Chem. Soc. 114, 10024 (1992)
V. Barone, M. Cossi, J. Tomasi, J. Chem. Phys. 107, 3210 (1997)
W.L. Jorgensen, J.K. Buckner, S. Boudon, J. Tirado-Rives, J. Chem. Phys. 89, 3742 (1988)
M.C.P. Lima, K. Coutinho, S. Canuto, W.R. Rocha, J. Phys. Chem. A 110, 7253 (2006)
M.E. Tuckerman, Statistical Mechanics: Theory and Molecular Simulation (Oxford Press, 2010)
A.R. da Cunha, E.L. Duarte, M.T. Lamy, K. Coutinho, Chem. Phys. 440, 69 (2014)
H.C. Georg, K. Coutinho, S. Canuto, J. Chem. Phys. 126, 034507 (2007)
S. Canuto, K. Coutinho, D. Trzesniak, Adv. Quantum Chem. 41, 161 (2002)
H.C. Georg, K. Coutinho, S. Canuto, Chem. Phys. Lett. 429, 119 (2006)
K. Coutinho, R. Rivelino, H.C. Georg, S. Canuto, in Computational Methods and Applications, edited by S. Canuto (Springer, 2008), p. 159
K. Coutinho, S. Canuto, DICE: A Monte Carlo program for molecular liquid simulations (University of São Paulo, 2003)
M. Allen, D. Tildesley, Computer Simulation of Liquids (Oxford Science Publications, Clarendon Press, 1989)
H.J.C. Berendsen, J.R. Grigera, T.P. Straatsma, J. Phys. Chem. 91, 6269 (1987)
W.L. Jorgensen, D.S. Maxwell, J. Tirado-Rives, J. Am. Chem. Soc. 118, 11225 (1996)
J. Pranata, S.G. Wierschke, W.L. Jorgensen, J. Am. Chem. Soc. 113, 2810 (1991)
C.M. Breneman, K.B. Wiberg, J. Comput. Chem. 11, 361 (1990)
K. Coutinho, H. Georg, T.L. Fonseca, V. Ludwig, S. Canuto, Chem. Phys. Lett. 437, 148 (2007)
P.D. Mitev, P.A. Bopp, J. Petreska, K. Coutinho, H. Ågren, L. Pejov, K. Hermansson, J. Chem. Phys. 138, 064503 (2013)
D.L. Silva, R.C. Barreto, E.G. Lacerda Jr., K. Coutinho, S. Canuto, Spectrochim. Acta A 119, 63 (2014)
M.D. Sevilla, B. Besler, A.O. Colson, J. Phys. Chem. 98, 2215 (1994)
H.Y. Chen, P.Y. Yang, H.F. Chen, C.L. Kao, L.W. Liao, J. Phys. Chem. B 118, 11137 (2014)
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Cornetta, L., Coutinho, K., Canuto, S. et al. Free energy barrier for dissociation of the guanosine monophosphate anion in water. Eur. Phys. J. D 70, 176 (2016). https://doi.org/10.1140/epjd/e2016-70155-0
Received:
Revised:
Published:
DOI: https://doi.org/10.1140/epjd/e2016-70155-0