Abstract

We report scattering experiments of multiphoton vibrationally excited SF6 molecules from graphite surfaces demonstrating ro-vibrational excitation in the collision. The beam scattering experiments were carried out at different initial kinematic conditions and as a function of the surface temperature. The energy transfer depends both on the initial state of the molecule and on the momentum transferred as well as on the temperature of the surface. The role of surface atomic corrugation is evidenced.

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References

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  1. P. L. Houston and R. P. Merrill, "Gas-Surface Interactions with Vibrationally Excited Molecules," Chem. Rev. 88, 657-671 (1988).
    [CrossRef]
  2. C. T. Rettner, D. J. Auerbach, J. C. Tully and A. W. Kleyn, "Chemical Dynamics at the Gas-Surface Interface," J. Phys. Chem. 100, 13021-13033 (1996).
    [CrossRef]
  3. M. B. Andersson and J. B. C. Pettersson, "Vibrational excitation of SF6 scattering from graphite," Chem. Phys. Lett. 250, 555-559 (1995).
    [CrossRef]
  4. E. R. Fischer, B. L. Kickel and P. B. Armentrout, "Collision-induced dissociation and charge transfer reactions of SFx + (x=1-5): Thermochemistry of sulfur fluoride ions and neutrals," J. Chem. Phys. 97, 4859- 4870 (1992).
    [CrossRef]
  5. S. Yamamoto, K. Mochiji and N. Mikami, "Trapping and low-energy extraction of photodissociated ions of SF6," Jpn. J. Appl. Phys. 34, L393-L395 (1995).
    [CrossRef]
  6. A. Boschetti, M. Zen, D. Bassi and M. Scotoni, "Thermal effects in collision-free infrared multiphoton absorption by SF6 and CF3Br," Chem. Phys. 87, 131-138 (1984).
    [CrossRef]
  7. C. Liedenbaum, S. Stolte and J. Reuss, "Multi-photon excitation of a beam of SF6 molecules pumped and probed by cw CO2 lasers," Chem. Phys. 122, 443-454 (1988).
    [CrossRef]
  8. A. Boschetti, A. Cagol, C. Corradi, R. Jacobs, M. Mazzola and S. Iannotta, "Energy transfer processes and molecular degrees of freedom in the collision of SF6 molecules with the GaSe (001) surface," Chem. Phys. 163, 179-191 (1992).
    [CrossRef]
  9. M. van Opbergen, A. Boschetti and S. Iannotta, "Energy transfer processes in the scattering of multiphoton excited SF6 from the (001) surface of GaSe," submitted to Surface Science.
  10. G. Scoles, Atomic and molecular beam methods (Oxford Univ. Press, New York - Oxford, 1988).
  11. M. B. N†g†rd, N. Markovi a and J. B. C. Pettersson, "Scattering and trapping dynamics of gas-surface interactions: Vibrational excitation of CF3Br on graphite," J. Chem. Phys. 109, 10350-10360 (1998).
    [CrossRef]
  12. S. Iannotta, C. Gravili, A. Boschetti, A. Cagol and M. Cacciatore, "Energy transfer processes and surface corrugation: a combined collision dynamics and experimental study of the Xe-GaSe (001) system," Chem. Phys. 194, 133-144 (1995).
    [CrossRef]
  13. S. Iannotta, G. Scoles and U. Valbusa, "Effect of surface atom vibrations on the diffraction of 1 H and 2 H beams from the basal plane of graphite," J. Phys. Chem. 89, 1914-1921 (1985).
    [CrossRef]

Other (13)

P. L. Houston and R. P. Merrill, "Gas-Surface Interactions with Vibrationally Excited Molecules," Chem. Rev. 88, 657-671 (1988).
[CrossRef]

C. T. Rettner, D. J. Auerbach, J. C. Tully and A. W. Kleyn, "Chemical Dynamics at the Gas-Surface Interface," J. Phys. Chem. 100, 13021-13033 (1996).
[CrossRef]

M. B. Andersson and J. B. C. Pettersson, "Vibrational excitation of SF6 scattering from graphite," Chem. Phys. Lett. 250, 555-559 (1995).
[CrossRef]

E. R. Fischer, B. L. Kickel and P. B. Armentrout, "Collision-induced dissociation and charge transfer reactions of SFx + (x=1-5): Thermochemistry of sulfur fluoride ions and neutrals," J. Chem. Phys. 97, 4859- 4870 (1992).
[CrossRef]

S. Yamamoto, K. Mochiji and N. Mikami, "Trapping and low-energy extraction of photodissociated ions of SF6," Jpn. J. Appl. Phys. 34, L393-L395 (1995).
[CrossRef]

A. Boschetti, M. Zen, D. Bassi and M. Scotoni, "Thermal effects in collision-free infrared multiphoton absorption by SF6 and CF3Br," Chem. Phys. 87, 131-138 (1984).
[CrossRef]

C. Liedenbaum, S. Stolte and J. Reuss, "Multi-photon excitation of a beam of SF6 molecules pumped and probed by cw CO2 lasers," Chem. Phys. 122, 443-454 (1988).
[CrossRef]

A. Boschetti, A. Cagol, C. Corradi, R. Jacobs, M. Mazzola and S. Iannotta, "Energy transfer processes and molecular degrees of freedom in the collision of SF6 molecules with the GaSe (001) surface," Chem. Phys. 163, 179-191 (1992).
[CrossRef]

M. van Opbergen, A. Boschetti and S. Iannotta, "Energy transfer processes in the scattering of multiphoton excited SF6 from the (001) surface of GaSe," submitted to Surface Science.

G. Scoles, Atomic and molecular beam methods (Oxford Univ. Press, New York - Oxford, 1988).

M. B. N†g†rd, N. Markovi a and J. B. C. Pettersson, "Scattering and trapping dynamics of gas-surface interactions: Vibrational excitation of CF3Br on graphite," J. Chem. Phys. 109, 10350-10360 (1998).
[CrossRef]

S. Iannotta, C. Gravili, A. Boschetti, A. Cagol and M. Cacciatore, "Energy transfer processes and surface corrugation: a combined collision dynamics and experimental study of the Xe-GaSe (001) system," Chem. Phys. 194, 133-144 (1995).
[CrossRef]

S. Iannotta, G. Scoles and U. Valbusa, "Effect of surface atom vibrations on the diffraction of 1 H and 2 H beams from the basal plane of graphite," J. Phys. Chem. 89, 1914-1921 (1985).
[CrossRef]

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Figures (3)

Fig. 1.
Fig. 1.

a) Normalised angular distributions of scattered SF6 molecules (Vbeam=520m/s) for three different surface temperatures. b) Distributions of SF6 beams scattered from the HOPG surface (Ts=178K) at different initial beam velocities. The arrows indicate the position of the incidence and specular angles (±40° respectively). The coloured signs on the degree scale of fig.1a show the angles calculated kinematically (see text).

Fig. 2.
Fig. 2.

a) Normalised angular distributions of laser multiphoton excited SF6 molecules scattered from the graphite surface (Ts=178K) at different initial beam velocities. b) Normalised intensity of the lobes for the laser induced scattering signals of two different beams as a function of the opto-thermal intensity of the incoming beam (see text). The open symbols represent the data obtained on the GaSe surface while the closed symbols show the results from the graphite surface. The lines are shown just to guide the eye.

Fig. 3.
Fig. 3.

Position of the maximum of the lobes (degrees from surface normal) as a function of the average beam velocity. The open symbols are for the laser induced angular distributions, while the closed symbols are from the results with the thermal beams. The angle of incidence is 40° (Ts=178K).

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