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Kinetics of atomic hydrogen+adsorbed Br reactions on Si(100) and Si(111) surfaces
The kinetics of adsorbed Br removal on Si(100) and Si(111) using atomic hydrogen are presented for surface temperatures from 50–560 °C. Both the surface H and Br coverages are measured in re...
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We present a Monte Carlo simulation study of adsorption on a plane solid surface from a model binary liquid mixture with a miscibility gap terminating at an upper critical solution temperature. The mo...

Quantum stochastic approach for molecule/surface scattering. I. Atom–phonon interactions

J. Chem. Phys. 99, 8229 (1993); doi:10.1063/1.465648

Issue Date: 15 November 1993

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Eric R. Bittner and John C. Light
The James Franck Institute and the Department of Chemistry, The University of Chicago, Chicago, Illinois 60637
We present a general, fully quantum mechanical theory for molecule surface scattering at finite temperature within the time dependent Hartree (TDH) factorization. We show the formal manipulations which reduce the total molecule–surface–bath Schrödinger equation into a form which is computationally convenient to use. Under the TDH factorization, the molecular portion of the wavefunction evolves according to a mean-field Hamiltonian which is dependent upon both time and temperature. The temporal and thermal dependence is due to stochastic and dissipative terms that appear in the Heisenberg equations of motion for the phonon operators upon averaging over the bath states. The resulting equations of motion are solved in one dimension self consistently using quantum wavepackets and the discrete variable representation. We compute energy transfer to the phonons as a function of surface temperature and initial energy and compare our results to results obtained using other mean-field models, namely an averaged mean-field model and a fully quantum model based upon a dissipative form of the quantum Liouville equation. It appears that the model presented here provides a better estimation of energy transfer between the molecule and the surface. The Journal of Chemical Physics is copyrighted by The American Institute of Physics.
History: Received 25 June 1993; accepted 10 August 1993
Permalink: http://link.aip.org/link/?JCPSA6/99/8229/1
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KEYWORDS and PACS

Keywords
PACS
  • 79.20.Nc
    Electron and ion emission by liquids and solids; impact phenomena Impact phenomena (including electron spectra and sputtering) Atom, molecule, and ion impact
  • 03.65.Nk
    Classical and quantum physics: mechanics and fields Quantum theory; quantum mechanics Nonrelativistic scattering theory
  • YEAR: 1993

PUBLICATION DATA

ISSN:
0021-9606 (print)   1089-7690 (online)
Publisher:
AIP is a member of CrossRef AIP

REFERENCES (42)
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  1. P. A. M. Dirac, Proc. Cambridge Philos. Soc. 26, 370 (1930).
  2. R. Alimi, R. B. Gerber, A. D. Hammerlich, R. Kosloff, and M. A. Ratner, J. Chem. Phys. 93, 6484 (1990).
  3. G. Wahnstrom, B. Carmeli, and H. Metiu, J. Chem. Phys. 88, 2474 (1988).
  4. S. Haug and H. Metiu, J. Chem. Phys. 97 (1992).
  5. R. Kosloff and C. Cerjan, J. Chem. Phys. 81, 3722 (1984).
  6. R. Kosloff and C. Cerjan, J. Chem. Phys. 90, 7556 (1989).
  7. C. Cerjan and R. Kosloff, Phys. Rev. B 34, 3832 (1985).
  8. E. B. Davies, Comm. Math. Phys. 39, 91 (1974).
  9. G. Linblad, Comm. Math. Phys. 48, 119 (1976).
  10. A. J. Cruz and B. Jackson, J. Chem. Phys. 91, 4985 (1985).
  11. B. Jackson and H. Metiu, J. Chem. Phys. 84, 3535 (1986).
  12. B. Jackson, J. Chem. Phys. 88, 1383 (1988).
  13. B. Jackson, J. Chem. Phys. 90, 140 (1989).
  14. B. Jackson, J. Chem. Phys. 92, 1458 (1990).
  15. B. Jackson, J. Chem. Phys. 94, 787 (1991).
  16. V. Bortolani, A. Franchini, and G. Santoro, in Dynamical Phenomena at Surfaces, Interfaces, and Superlattices, edited by F. Nizzoli, K. H. Rieder, and R. F. Willis (Springer-Verlag, Berlin, 1985).
  17. V. Buch, J. Chem. Phys. 86, 3627 (1987).
  18. V. Buch, J. Chem. Phys. 91, 3788 (1987).
  19. V. Buch, J. Chem. Phys. 91, 4974 (1989).
  20. K. B. Whaley and A. Bennett, J. Chem. Phys. 95, 6136 (1991).
  21. J. R. Manson, Phys. Rev. B 43, 6924 (1990).
  22. B. H. Choi and R. T. Poe, J. Chem. Phys. 83, 1344 (1985).
  23. B. H. Choi, Z. B. Giivenc, and N. L. Liu, Phys. Rev. B 42, 3907 (1990).
  24. F. Haake and R. Reibold, Phys. Rev. A 32, 2462 (1985).
  25. P. Ullersma, in Scattering in Condensed Matter, edited by W. Eisenmenger (Springer-Verlag, Berlin, 1984).
  26. S. van Smaalen and T. F. George, J. Chem. Phys. 87, 5504 (1987).
  27. K. Lindenberg and B. J. West, Nonequilibrium Statistical Mechanics of Open and Closed Systems (VCH, NewYork, 1990).
  28. G. W. Ford, M. Kac, and P. Mazur, J. Math. Phys. 6, 504 (1965).
  29. C. W. Gardiner, Handbook of Stochastic Methods (Springer-Verlag, Berlin, 1990).
  30. K. Y. R. Billah and M. Shinozuka, Phys. Rev. A 42, 7492 (1992).
  31. W. H. Press, B. Flannery, S. A. Teukolsky, and W. T. Vetterling, Numerical Recipies (Cambridge University, Cambridge, 1986).
  32. R. Heather and H. Metiu, J. Chem. Phys. 86, 5009 (1987).
  33. M. D. Feit, J. A. Fleck, and A. Steiger, J. Comput. Phys. 47, 412 (1982).
  34. M. D. Feit and J. A. Fleck, J. Chem. Phys. 78, 301 (1984).
  35. C. Leforistier et al., J. Comput. Phys. 94, 59 (1991).
  36. J. C. Light, I. P. Hamilton, and J. V. Lill, J. Chem. Phys. 85, 1400 (1985).
  37. S. E. Choi and J. C. Light, J. Chem. Phys. 90, 2589 (1990).
  38. J. C. Light, R. Whitnell, T. J. Park, and S. E. Choi, in Supercomputer Algorithms for Reactivity, Dynamics, and Kinetics of Small Molecules, edited by A. Lagana (Kluwer, Dordrecht, 1989), p. 187.
  39. K. D. Gibson, C. Cerjan, J. C. Light, and S. J. Sibener, J. Chem. Phys. 88, 7911 (1988).
  40. K. D. Gibson and S. J. Sibener, J. Chem. Phys. 88, 7893 (1988).
  41. R. B. Gerber, V. Buch, and M. A. Ratner, J. Chem. Phys. 77, 3022 (1982).
  42. R. B. Gerber and M. A. Ratner, Adv. Chem. Phys. 70, 97 (1988).

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