Abstract
By making use of a Grid enabled ab initio molecular simulator we have tackled the a priori study of the N2(\({}^1{\Sigma}_g^+\)) + N2(\({}^1{\Sigma}_g^+\)) process. A detailed analysis of the results obtained from high level ab initio (Coupled Cluster) calculation of the electronic structure of N4 for a large number of nuclear geometries has singled out the fact that Coupled Cluster calculations are insufficiently accurate when the internuclear distances of the approaching N2 diatoms are stretched, because in such cases the wavefunction of the N4 system cannot be properly described by a single determinant. For this reason we have carried out Multi Reference calculations (using the same basis set) for a large number of the nuclear geometries considered for the Coupled Cluster study. Then, a 4-atoms global potential energy surface has been worked out for use in dynamics calculations.
Access this chapter
Tax calculation will be finalised at checkout
Purchases are for personal use only
Preview
Unable to display preview. Download preview PDF.
References
Nesbitt, D.J., van der Avoird, A.: Rovibrational states of the H2O-H2 complex: An ab initio calculation. J. Chem. Phys. 134, 44314 (2011)
Albertí, M., Faginas Lago, N., Pirani, F.: Benzene water interaction: From gaseous dimers to solvated aggregates. Chem. Phys. 339, 232–239 (2012)
Hinde, R.J.: A six-dimensional H2H2 potential energy surface for bound state spectroscopy. J. Chem. Phys. 128, 154308 (2008)
Ceballos, A., Garcia, E., Rodriguez, A., Laganà, A.: Quasiclassical kinetics of the H2 + H2 reaction and dissociation. J. Chem. Phys. 105(10), 1797–1804 (2001)
Capitelli, M.: Non-equilibrium vibrational kinetics. Springer, Berlin (1986)
Armenise, I., Capitelli, M., Garcia, E., Gorse, C., Laganà, A., Longo, S.: Deactivation dynamics of vibrationally excited nitrogen molecules by nitrogen atoms. Effects on non-equilibrium vibrational distribution and dissociation rates of nitrogen under electrical discharges. Chem. Phys. Lett. 200, 597 (1992)
Knauth, D.C., Andersson, B.G., McCandliss, S.R., Moos, H.W.: The Interstellar N2 Abundance toward HD 124314 from Far-Ultraviolet Observations. Nature 429, 636 (2004)
Raich, J.C., Gillis, N.S.: The anisotropic interaction between nitrogen molecules from solid state data. J. Chem. Phys. 66, 846 (1977)
MacRury, T.B., Steele, W.A., Berne, B.J.: Intermolecular potential models for anisotropic molecules, with applications to N2, CO2, and benzene. J. Chem. Phys. 64, 1288 (1976)
Cheung, P.S.Y., Powles, J.G.: The properties of liquid nitrogen V. Computer simulation with quadrupole interaction. Mol. Phys. 32, 1383 (1976)
Cheung, P.S.Y., Powles, J.G.: The properties of liquid nitrogen. Mol. Phys. 30, 921 (1975)
Evans, D.J.: Transport properties of homonuclear diatomics I. Dilute gases. Mol. Phys. 34, 103 (1977)
Cappelletti, D., Vecchiocattivi, F., Pirani, F., Heck, E.L., Dickinson, A.S.: An Intermolecular potential for Nitrogen from a multi-property analysis. Mol. Phys. 93, 485 (1998)
Aquilanti, V., Bartolomei, M., Cappelletti, D., Caramona-Novillo, E., Pirani, F.: The N2-N2 system: An experimental potential energy surface and calculated rotovibrational levels of the molecular nitrogen dimer. J. Chem. Phys. 93, 485 (1998)
Gomez, L., Bussery-Honvault, B., Cauchy, T., Bartolomei, M., Cappelletti, D., Pirani, F.: Global fits of new intermolecular ground state potential energy surfaces for N2-H2 and N2-N2 van der waals dimers. Chem. Phys. Lett. 445, 99–107 (2007)
van der Avoid, A., Wormer, P.E.S., Jansen, A.P.J.: An improved intermolecular potential for nitrogen. J. Chem. Phys. 84, 1629–1635 (1986)
Cappelletti, D., Vecchiocattivi, F., Pirani, F., McCourt, F.R.W.: Glory structure in the N2-N2 total integral scattering cross section. A test for the intermolecular potential energy surface. Chem. Phys. Lett. 248, 237–243 (1996)
Huo, S.W.M., Green, S.: Quantum calculations for rotational energy transfer in nitrogen molecule collisions. J. Chem. Phys. 104, 7572–7589 (1996)
Stallcop, J.R., Partridge, H.: The N2-N2 potential energy surface. Chem. Phys. Lett. 281, 212–220 (1997)
Wada, A., Kanamori, H., Iwata, S.: Ab Initio MO studies of van der waals molecule (N2)2: Potential energy surface and internal motion. J. Chem. Phys. 109, 9434–9438 (1998)
Couronne, O., Ellinger, Y.A.: An ab initio and DFT study of (N2)2 dimers. Chem. Phys. Lett. 306, 71–77 (1999)
Leonhard, K., Deiters, U.K.: Monte Carlo Simulations of Nitrogen Using an Ab Initio Potential. Mol. Phys. 100, 2571–2585 (2002)
Karimi Jafari, M.H., Maghari, A., Shahbazian, S.: An improved ab initio potential energy surface for N2-N2. Chem. Phys. 314, 249–262 (2005)
Laganà, A., Riganelli, A., Gervasi, O.: On the structuring of the computational chemistry Virtual Organization COMPCHEM. In: Gavrilova, M.L., Gervasi, O., Kumar, V., Tan, C.J.K., Taniar, D., Laganá, A., Mun, Y., Choo, H. (eds.) ICCSA 2006. LNCS, vol. 3980, pp. 665–674. Springer, Heidelberg (2006)
The European Grid Initiative, http://www.egi.com (last access January 13, 2013)
Laganà, A.: Towards a grid based universal molecular simulator. In: Laganà, A., Lendvay, G. (eds.). Kluwer (2004)
Costantini, A., Gervasi, O., Manuali, C., Faginas Lago, N., Rampino, S., Laganà, A.: COMPCHEM: progress towards gems a grid empowered molecular simulator and beyond. Journal of Grid Computing 8, 571–586 (2010)
Rampino, S., Monari, A., Rossi, E., Evangelisti, S., Laganà, A.: Chem. Phys. 398, 192 (2012)
Laganá, A., Balucani, N., Crocchianti, S., Casavecchia, P., Garcia, E., Saracibar, A.: An extension of the molecular simulator GEMS to calculate the signal of crossed beam experiments. In: Murgante, B., Gervasi, O., Iglesias, A., Taniar, D., Apduhan, B.O. (eds.) ICCSA 2011, Part III. LNCS, vol. 6784, pp. 453–465. Springer, Heidelberg (2011)
Verdicchio, M., Pacifici, L., Laganà, A.: Grid enabled high level ab initio electronic structure calculations for the N2 + N2 exchange reaction. In: Murgante, B., Gervasi, O., Misra, S., Nedjah, N., Rocha, A.M.A.C., Taniar, D., Apduhan, B.O. (eds.) ICCSA 2012, Part I. LNCS, vol. 7333, pp. 371–386. Springer, Heidelberg (2012)
Møller, C., Plesset, M.S.: Note on an Approximation Treatment for Many-Electron Systems. Phys. Rev. 46, 618 (1934)
Boys, S.F., Bernardi, F.: The calculation of small molecular interactions by the differences of separate total energies. Some procedures with reduced errors. Mol. Phys. 19, 553–566 (1970)
Feller, D.: The Role of Databases in Support of Computational Chemistry Calculations. J. Chem. Phys. 17, 1571–1586 (1996)
Schuchardt, K., Didier, B., Elsethagen, T., Sun, L., Gurumoorthi, V., Chase, J., Li, J., Windus, T.: Basis Set Exchange: A Community Database for Computational Sciences. J. Chem Inf. Model. 47, 1045–1052 (2007)
Piecuch, P., Kucharski, S.A., Kowalski, K., Musial, M.: Efficient computer implementation of the renormalized coupled-cluster methods: The R-CCSD[T], R-CCSD(T), CR-CCSD[T], and CR-CCSD(T) approaches. Comput. Phys. Comm. 149, 71–96 (2002)
Bentz, J.L., Olson, R.M., Gordon, M.S., Schmidt, M.W., Kendall, R.A.: Coupled cluster algorithms for networks of shared memory parallel processors. Comput. Phys. Comm. 176, 589–600 (2007)
Olson, R.M., Bentz, J.L., Kendall, R.A., Schmidt, M.W., Gordon, M.S.: A novel approach to parallel coupled cluster calculations: Combining distributed and shared memory techniques for modern cluster based systems. J. Comput. Theo. Chem. 3, 1312–1328 (2007)
Schmidt, M.W., Baldridge, K.K., Boatz, J.A., Elbert, S.T., Gordon, M.S., Jensen, J.J., Koseki, S., Matsunaga, N., Nguyen, K.A., Su, S., Windus, T.L., Dupuis, M., Montgomery, J.A.: General atomic and molecular electronic structure system. J. Comp. Chem. 14, 1347–1363 (1993)
Gordon, M.S., Schmidt, M.W.: Theory and Applications of Computational Chemistry, the first forty years (2005)
Hay, P.J., Pack, R.T., Martin, R.L.: Electron correlation effects on the N2-N2 interaction. J. Chem. Phys. 81, 1360–1372 (1984)
http://www.cineca.it (last access January 21, 2013)
Sorbie, K.S., Murrell, J.N.: Analytical potentials for triatomic molecules from spectroscopic data. Mol. Phys. 52, 1387 (1975)
Aguado, A., Tablero, C., Paniagua, M.: Global fit of ab initio potential energy surfaces: II.1. tetraatomic systems ABCD. Comput. Phys. Comm. 134, 97 (2001)
Garcia, E., Saracibar, A., Gomez-Carrasco, S., Laganà, A.: Modelling the global potential energy surface of the N + N2 reaction from ab initio data. Phys. Chem. Chem. Phys. 10, 2552–2558 (2008)
Caridade, P.J.S.B., Galvao, B.R.L., Varandas, A.J.C.: Quasiclassical Trajectory Study of Atom-Exchange and Vibrational Relaxation Processes in Collisions of Atomic and Molecular Nitrogen. J. Phys. Chem. A 114, 6063–6070 (2010)
Baerends, E.J., Ellis, D.E., Ros, P.: Chem. Phys. 2, 41 (1973)
Ziegler, T., Snijders, J.G., Baerends, E.J.: J. Chem. Phys. 74, 1271 (1981)
Hirao, K.: Chem. Phys. Lett. 190, 374 (1992)
Hirao, K.: Int. J. Quant. Chem. S26, 517 (1992)
Author information
Authors and Affiliations
Editor information
Editors and Affiliations
Rights and permissions
Copyright information
© 2013 Springer-Verlag Berlin Heidelberg
About this paper
Cite this paper
Pacifici, L., Verdicchio, M., Laganà, A. (2013). Multi Reference versus Coupled Cluster ab Initio Calculations for the N2 + N2 Reaction Channels. In: Murgante, B., et al. Computational Science and Its Applications – ICCSA 2013. ICCSA 2013. Lecture Notes in Computer Science, vol 7971. Springer, Berlin, Heidelberg. https://doi.org/10.1007/978-3-642-39637-3_3
Download citation
DOI: https://doi.org/10.1007/978-3-642-39637-3_3
Publisher Name: Springer, Berlin, Heidelberg
Print ISBN: 978-3-642-39636-6
Online ISBN: 978-3-642-39637-3
eBook Packages: Computer ScienceComputer Science (R0)