Nuclear quantum effects and hydrogen bonding in liquids

Journal of the American Chemical Society

Volumn 125, Issue 30, 2003, Pages 8992-8993

  Raugei, Simone ^a   Klein, Michael L ^b  

^a SISSA   (Italy)

^b UNIVERSITY OF PENNSYLVANIA   (United States)

Author keywords

[No Author keywords available]

Indexed keywords

HYDROFLUORIC ACID;

ARTICLE; HYDROGEN BOND; LIQUID; MOLECULAR DYNAMICS; MOLECULAR INTERACTION; QUANTUM MECHANICS; SIMULATION; TEMPERATURE DEPENDENCE;

HYDROFLUORIC ACID; HYDROGEN BONDING; NUCLEIC ACIDS; PROTEINS; QUANTUM THEORY;

EID: 0042367654     PISSN: 00027863     EISSN: None     Source Type: Journal    
DOI: 10.1021/ja0351995     Document Type: Article

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20. In the present DFT calculations, we have utilized Troullier-Martins pseudopotentials [Troullier, N.; Martins, J. L. Phys. Rev. B 1991, 43, 1993] to describe the atomic core of F atoms and a von Barth-Car pseudopotential [see, e.g., ref 15] for hydrogens. The valence wave functions have been expanded in plane-waves up to an energy cutoff of 70 Ry. We have employed the Becke, Lee, Parr, and Yang exchange and correlation functional (BLYP) [Becke, A. D. Phys. Rev. A 1988, 38, 3098. Lee, C.; Yang, W.; Parr, R. G. Phys. Rev. B 1988, 37, 7851, which yield excellent results for both water and HF. The simulation cell consists of 54 HF molecules enclosed in a cubic box at the experimental density [Honda, K.; Kitaura, K.; Nishimoto, K. Bull. Chem. Soc. Jpn. 1992, 65, 3122]. The starting configuration for the simulations has been taken from previous studies. The PI has been represented by 16 discrete beads. The equations of motion have been integrated with a time step of 0.121 fs using 800 au as a fictitious electronic mass. The systems have been equilibrated at 290 K for 3 ps, and then the trajectories were collected for about 9 ps. To guarantee adiabaticity of the PI simulation, thermostats have been also applied to electrons. All of the calculations have been performed by using the CPMD code [Hutter, J.; et al. CPMD (IBM Zurich Research Laboratory and MPI für Festkörperforschung, 2002)].
21. In the present DFT calculations, we have utilized Troullier-Martins pseudopotentials [Troullier, N.; Martins, J. L. Phys. Rev. B 1991, 43, 1993] to describe the atomic core of F atoms and a von Barth-Car pseudopotential [see, e.g., ref 15] for hydrogens. The valence wave functions have been expanded in plane-waves up to an energy cutoff of 70 Ry. We have employed the Becke, Lee, Parr, and Yang exchange and correlation functional (BLYP) [Becke, A. D. Phys. Rev. A 1988, 38, 3098. Lee, C.; Yang, W.; Parr, R. G. Phys. Rev. B 1988, 37, 7851, which yield excellent results for both water and HF. The simulation cell consists of 54 HF molecules enclosed in a cubic box at the experimental density [Honda, K.; Kitaura, K.; Nishimoto, K. Bull. Chem. Soc. Jpn. 1992, 65, 3122]. The starting configuration for the simulations has been taken from previous studies. The PI has been represented by 16 discrete beads. The equations of motion have been integrated with a time step of 0.121 fs using 800 au as a fictitious electronic mass. The systems have been equilibrated at 290 K for 3 ps, and then the trajectories were collected for about 9 ps. To guarantee adiabaticity of the PI simulation, thermostats have been also applied to electrons. All of the calculations have been performed by using the CPMD code [Hutter, J.; et al. CPMD (IBM Zurich Research Laboratory and MPI für Festkörperforschung, 2002)].
22. In the present DFT calculations, we have utilized Troullier-Martins pseudopotentials [Troullier, N.; Martins, J. L. Phys. Rev. B 1991, 43, 1993] to describe the atomic core of F atoms and a von Barth-Car pseudopotential [see, e.g., ref 15] for hydrogens. The valence wave functions have been expanded in plane-waves up to an energy cutoff of 70 Ry. We have employed the Becke, Lee, Parr, and Yang exchange and correlation functional (BLYP) [Becke, A. D. Phys. Rev. A 1988, 38, 3098. Lee, C.; Yang, W.; Parr, R. G. Phys. Rev. B 1988, 37, 7851, which yield excellent results for both water and HF. The simulation cell consists of 54 HF molecules enclosed in a cubic box at the experimental density [Honda, K.; Kitaura, K.; Nishimoto, K. Bull. Chem. Soc. Jpn. 1992, 65, 3122]. The starting configuration for the simulations has been taken from previous studies. The PI has been represented by 16 discrete beads. The equations of motion have been integrated with a time step of 0.121 fs using 800 au as a fictitious electronic mass. The systems have been equilibrated at 290 K for 3 ps, and then the trajectories were collected for about 9 ps. To guarantee adiabaticity of the PI simulation, thermostats have been also applied to electrons. All of the calculations have been performed by using the CPMD code [Hutter, J.; et al. CPMD (IBM Zurich Research Laboratory and MPI für Festkörperforschung, 2002)].
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29. These values should be compared to the value 0,932 A computed at the same level of theory for the monomer in vacuo. The experimental value is 0.917 Å [Mason, M. G.; von Holle, W. G.; Robinson, D. W. J. Chem. Phys. 1971, 54, 3491].
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36. It is also worth observing that the F⋯F intrachain distance computed in both C and Q compares well with the distance measured for liquid DF at 293 K (2.56 Å) and 300 K (2.53 Å) crystalline DF at 85 K (2.49).
37. The largest source of error is likely the intrinsic error due to the use of the BLYP functional. Although DFT/BLYP calculations give good structural properties of H-bonded systems, it is not clear if polarization effects are equally well reproduced. However, any error should have the same influence in both C and Q simulations. Another error could be due to the small size of the simulation cell. Here, we have checked the influence of system size by performing simulations on a smaller simulation cell (27 molecules) with a smaller number of beads (8) to represent the PI. The overall picture is the same as the one discussed herein. Thus, the PI calculations are likely sufficiently well converged with regard to the (short-range) hydrogen-bonding patterns. We have also checked for size effects on the computed dipole moment without observing any relevant dependence (the average dipole moment difference between cells composed by 27 and 54 molecules is 0.04 D). Furthermore, the average net dipole moment of the entire cell is negligible (about 0.2 D) in all cases. Hence, we can rule out strong dipole-dipole interactions between the cell and its images.