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.

© 1999 Optical Society of America

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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. Någård, N. Marković, 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 1H and 2H beams from the basal plane of graphite,” J. Phys. Chem. 89, 1914–1921 (1985).
    [Crossref]

1998 (1)

M. B. Någård, N. Marković, 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]

1996 (1)

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]

1995 (3)

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

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]

1992 (2)

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]

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]

1988 (2)

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

1985 (1)

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

1984 (1)

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]

Andersson, M. B.

M. B. Andersson and J. B. C. Pettersson, “Vibrational excitation of SF6 scattering from graphite,” Chem. Phys. Lett. 250, 555–559 (1995).
[Crossref]

Armentrout, P. B.

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]

Auerbach, D. J.

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]

Bassi, D.

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]

Boschetti, A.

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]

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]

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]

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.

Cacciatore, M.

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]

Cagol, A.

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]

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]

Corradi, C.

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]

Fischer, E. R.

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]

Gravili, C.

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]

Houston, P. L.

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

Iannotta, S.

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]

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]

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

Jacobs, R.

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]

Kickel, B. L.

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]

Kleyn, A. W.

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]

Liedenbaum, C.

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]

Markovic, N.

M. B. Någård, N. Marković, 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]

Mazzola, M.

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]

Merrill, R. P.

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

Mikami, N.

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]

Mochiji, K.

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]

Någård, M. B.

M. B. Någård, N. Marković, 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]

Pettersson, J. B. C.

M. B. Någård, N. Marković, 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]

M. B. Andersson and J. B. C. Pettersson, “Vibrational excitation of SF6 scattering from graphite,” Chem. Phys. Lett. 250, 555–559 (1995).
[Crossref]

Rettner, C. T.

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]

Reuss, J.

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]

Scoles, G.

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

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

Scotoni, M.

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]

Stolte, S.

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]

Tully, J. C.

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]

Valbusa, U.

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

van Opbergen, M.

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.

Yamamoto, S.

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]

Zen, M.

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]

Chem. Phys. (4)

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]

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]

Chem. Phys. Lett. (1)

M. B. Andersson and J. B. C. Pettersson, “Vibrational excitation of SF6 scattering from graphite,” Chem. Phys. Lett. 250, 555–559 (1995).
[Crossref]

Chem. Rev. (1)

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

J. Chem. Phys. (2)

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]

M. B. Någård, N. Marković, 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]

J. Phys. Chem. (2)

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

Jpn. J. Appl. Phys. (1)

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]

Other (2)

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).

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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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