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Volumn 282, Issue 5387, 1998, Pages 265-268

The chemistry of water on alumina surfaces: Reaction dynamics from first principles

Author keywords

[No Author keywords available]

Indexed keywords

ALUMINUM OXIDE; WATER;

EID: 0032500725     PISSN: 00368075     EISSN: None     Source Type: Journal    
DOI: 10.1126/science.282.5387.265     Document Type: Article
Times cited : (531)

References (41)
  • 7
    • 4243553426 scopus 로고
    • The gradient-corrected exchange-correlation [Bernstein, Lee, Yang, and Primakoff (BLYP)] functional used here is from A. D. Becke [Phys. Rev. A 38, 3098 (1988)] and C. Lee, W. Yang, and R. Parr [Phys. Rev. B 37, 785 (1988)]. Norm-conserving numerical pseudo-potentials were generated for Al and O with the procedure of N. Troullier and J. L. Martins [ibid. 43, 1993 (1991)], and a local analytic pseudopotential was derived for H. This is essentially a softened Coulomb potential with a core radius of 0.25 atomic units. Electron wave functions are expanded in a plane-wave basis set with an energy cutoff of 70 rydbergs (Ry). We used the Car-Parrinello Molecular Dynamics code in the parallelized 2.5 version (developed by J. Hutter and copyrighted by IBM, Armonk, NY). All calculations were performed on a 32-node IBM RS6000 SP at the IBM Watson Research Laboratory (Yorktown Heights, NY).
    • (1988) Phys. Rev. A , vol.38 , pp. 3098
    • Becke, A.D.1
  • 8
    • 0345491105 scopus 로고
    • The gradient-corrected exchange-correlation [Bernstein, Lee, Yang, and Primakoff (BLYP)] functional used here is from A. D. Becke [Phys. Rev. A 38, 3098 (1988)] and C. Lee, W. Yang, and R. Parr [Phys. Rev. B 37, 785 (1988)]. Norm-conserving numerical pseudo-potentials were generated for Al and O with the procedure of N. Troullier and J. L. Martins [ibid. 43, 1993 (1991)], and a local analytic pseudopotential was derived for H. This is essentially a softened Coulomb potential with a core radius of 0.25 atomic units. Electron wave functions are expanded in a plane-wave basis set with an energy cutoff of 70 rydbergs (Ry). We used the Car-Parrinello Molecular Dynamics code in the parallelized 2.5 version (developed by J. Hutter and copyrighted by IBM, Armonk, NY). All calculations were performed on a 32-node IBM RS6000 SP at the IBM Watson Research Laboratory (Yorktown Heights, NY).
    • (1988) Phys. Rev. B , vol.37 , pp. 785
    • Lee, C.1    Yang, W.2    Parr, R.3
  • 9
    • 33645426115 scopus 로고
    • The gradient-corrected exchange-correlation [Bernstein, Lee, Yang, and Primakoff (BLYP)] functional used here is from A. D. Becke [Phys. Rev. A 38, 3098 (1988)] and C. Lee, W. Yang, and R. Parr [Phys. Rev. B 37, 785 (1988)]. Norm-conserving numerical pseudo-potentials were generated for Al and O with the procedure of N. Troullier and J. L. Martins [ibid. 43, 1993 (1991)], and a local analytic pseudopotential was derived for H. This is essentially a softened Coulomb potential with a core radius of 0.25 atomic units. Electron wave functions are expanded in a plane-wave basis set with an energy cutoff of 70 rydbergs (Ry). We used the Car-Parrinello Molecular Dynamics code in the parallelized 2.5 version (developed by J. Hutter and copyrighted by IBM, Armonk, NY). All calculations were performed on a 32-node IBM RS6000 SP at the IBM Watson Research Laboratory (Yorktown Heights, NY).
    • (1991) Phys. Rev. B , vol.43 , pp. 1993
    • Troullier, N.1    Martins, J.L.2
  • 10
    • 85081422836 scopus 로고    scopus 로고
    • note
    • In the MD runs, a value of 400 au was used for the fictitious electron mass of the Car-Parrinello Lagrangian multipliers (6), and each hydrogen molecule was replaced by deuterium to improve the separation between electronic and ionic degrees of freedom. The time step in the Verlet algorithm for the integration of the equations of motions was ∼0.1 fs.
  • 11
    • 85081423699 scopus 로고    scopus 로고
    • Reaction Dynamics
    • The importance of chemical reaction dynamics in general has recently been highlighted in a special issue of Science [Reaction Dynamics, Science 279, 1875-1895 (1998)].
    • (1998) Science , vol.279 , pp. 1875-1895
  • 13
    • 0030782736 scopus 로고    scopus 로고
    • V. E. Puchin et al., Surf. Sci. 370, 190 (1997); J. Ahn and J. W. Rabalais, ibid. 388, 121 (1997).
    • (1997) Surf. Sci. , vol.370 , pp. 190
    • Puchin, V.E.1
  • 14
    • 0031244978 scopus 로고    scopus 로고
    • V. E. Puchin et al., Surf. Sci. 370, 190 (1997); J. Ahn and J. W. Rabalais, ibid. 388, 121 (1997).
    • (1997) Surf. Sci. , vol.388 , pp. 121
    • Ahn, J.1    Rabalais, J.W.2
  • 16
    • 4243266947 scopus 로고
    • See, for example, M. Causa, R. Dovesi, C. Pisani, C. Roetti, ibid. 215, 259 (1989); I. Manassidis, A. De Vita, M. J. Gillan, Surf. Sci. Lett. 285, L517 (1993); I. Frank, D. Marx, M. Parrinello, J. Chem. Phys. 104, 8143 (1996).
    • (1989) Surf. Sci. , vol.215 , pp. 259
    • Causa, M.1    Dovesi, R.2    Pisani, C.3    Roetti, C.4
  • 17
    • 0027576430 scopus 로고
    • See, for example, M. Causa, R. Dovesi, C. Pisani, C. Roetti, ibid. 215, 259 (1989); I. Manassidis, A. De Vita, M. J. Gillan, Surf. Sci. Lett. 285, L517 (1993); I. Frank, D. Marx, M. Parrinello, J. Chem. Phys. 104, 8143 (1996).
    • (1993) Surf. Sci. Lett. , vol.285
    • Manassidis, I.1    De Vita, A.2    Gillan, M.J.3
  • 18
    • 0000543828 scopus 로고    scopus 로고
    • See, for example, M. Causa, R. Dovesi, C. Pisani, C. Roetti, ibid. 215, 259 (1989); I. Manassidis, A. De Vita, M. J. Gillan, Surf. Sci. Lett. 285, L517 (1993); I. Frank, D. Marx, M. Parrinello, J. Chem. Phys. 104, 8143 (1996).
    • (1996) J. Chem. Phys. , vol.104 , pp. 8143
    • Frank, I.1    Marx, D.2    Parrinello, M.3
  • 19
    • 0030879486 scopus 로고    scopus 로고
    • J. M. McHale, A. Auroux, A. J. Perrotta, A. Navrotsky, Science 277, 788 (1997). For earlier work, see P. A. Thiel and T. E. Madey, Surf. Sci. Rep. 7, 211 (1987) and references therein.
    • (1997) Science , vol.277 , pp. 788
    • McHale, J.M.1    Auroux, A.2    Perrotta, A.J.3    Navrotsky, A.4
  • 20
    • 0142055513 scopus 로고
    • and references therein
    • J. M. McHale, A. Auroux, A. J. Perrotta, A. Navrotsky, Science 277, 788 (1997). For earlier work, see P. A. Thiel and T. E. Madey, Surf. Sci. Rep. 7, 211 (1987) and references therein.
    • (1987) Surf. Sci. Rep. , vol.7 , pp. 211
    • Thiel, P.A.1    Madey, T.E.2
  • 23
    • 85081421326 scopus 로고    scopus 로고
    • note
    • 2O coverage dependence and phenomena such as collective effects and surface diffusion.
  • 24
    • 0030129363 scopus 로고    scopus 로고
    • J. Goniakowski and M. J. Gillan, Surf. Sci. 350, 145 (1996); P. J. D. Lindan, N. M. Harrison, J. M. Holdender, M. J. Gillan, Chem. Phys. Lett. 261, 246 (1996); P. J. D. Lindan, N. M. Harrison, M. J. Gillan, Phys. Rev. Lett. 80, 762 (1998).
    • (1996) Surf. Sci. , vol.350 , pp. 145
    • Goniakowski, J.1    Gillan, M.J.2
  • 26
    • 11544350240 scopus 로고    scopus 로고
    • J. Goniakowski and M. J. Gillan, Surf. Sci. 350, 145 (1996); P. J. D. Lindan, N. M. Harrison, J. M. Holdender, M. J. Gillan, Chem. Phys. Lett. 261, 246 (1996); P. J. D. Lindan, N. M. Harrison, M. J. Gillan, Phys. Rev. Lett. 80, 762 (1998).
    • (1998) Phys. Rev. Lett. , vol.80 , pp. 762
    • Lindan, P.J.D.1    Harrison, N.M.2    Gillan, M.J.3
  • 28
    • 34547809547 scopus 로고
    • s distance, and the average constraint forces were determined from constant temperature simulations [S. Nosé, J. Chem. Phys. 81, 511 (1984); W. G. Hoover, Phys. Rev. A 31, 1695 (1985)] of at least 0.2 ps.
    • (1984) J. Chem. Phys. , vol.81 , pp. 511
    • Nosé, S.1
  • 29
    • 0001538909 scopus 로고
    • of at least 0.2 ps
    • s distance, and the average constraint forces were determined from constant temperature simulations [S. Nosé, J. Chem. Phys. 81, 511 (1984); W. G. Hoover, Phys. Rev. A 31, 1695 (1985)] of at least 0.2 ps.
    • (1985) Phys. Rev. A , vol.31 , pp. 1695
    • Hoover, W.G.1
  • 32
    • 85081421448 scopus 로고    scopus 로고
    • note
    • The temperature was not controlled but was increased slowly from ∼100 to ∼350 K. The system was then allowed to evolve for a time interval of >1 ps. The average temperature was 250 K.
  • 34
    • 85081423466 scopus 로고    scopus 로고
    • note
    • Vibrational frequencies were estimated from the power spectra of the (partial) velocity-velocity auto-correlation functions and were rescaled to account for the fictitious electronic mass and the different mass used for the proton.
  • 35
    • 0342757079 scopus 로고
    • V. I. Lygin and I. S. Muzyka, Russ. J. Phys. Chem. 69, 1829 (1995); A. Tsyganenko and P. Mardilovich, J. Chem. Soc. Faraday Trans. 92, 4843 (1996).
    • (1995) Russ. J. Phys. Chem. , vol.69 , pp. 1829
    • Lygin, V.I.1    Muzyka, I.S.2
  • 40
    • 36549097199 scopus 로고
    • C. Morterra, G. Ghiotti, E. Garrone, F. Boccuzzi, J. Chem. Soc. Faraday Trans. 1 72, 2722 (1976); J. G. Chen, J. E. Crowell, J. T. Yates, J. Chem. Phys. 84, 5906 (1986); V. Coustet and J. Jupille, Surf. Sci. 307, 1161 (1994).
    • (1986) J. Chem. Phys. , vol.84 , pp. 5906
    • Chen, J.G.1    Crowell, J.E.2    Yates, J.T.3
  • 41
    • 0028406780 scopus 로고
    • C. Morterra, G. Ghiotti, E. Garrone, F. Boccuzzi, J. Chem. Soc. Faraday Trans. 1 72, 2722 (1976); J. G. Chen, J. E. Crowell, J. T. Yates, J. Chem. Phys. 84, 5906 (1986); V. Coustet and J. Jupille, Surf. Sci. 307, 1161 (1994).
    • (1994) Surf. Sci. , vol.307 , pp. 1161
    • Coustet, V.1    Jupille, J.2


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