Combined crossed molecular beams and abinitio investigation of the formation of carbon-bearing molecules in the interstellar medium via neutral–neutral reactions

(Note: The full text of this document is currently only available in the PDF Version )

R. I. Kaiser, C. Ochsenfeld, D. Stranges, M. Head-Gordon and ¶ Y. T. Lee


Abstract

The crossed molecular beams reaction of atomic carbon C(3Pj) with hydrogen sulfide, H2S, allene, H2CCCH2, the vinyl radical, C2H3, and deuteroacetylene, C2HD, have been studied at different collision energies up to 42.2 kJ mol-1 and combined with high level abinitio calculations. All reactions are barrier-less and are dominated by a carbon–hydrogen exchange to form thioformyl (HCS), butatrienyl (HCCCCH2), C3H2 isomer(s), and deuteriated tricarbon hydride(s). This carbon–hydrogen replacement channel represents a one-step alternative reaction pathway to competing ion–molecule reactions to form complex, carbon-bearing molecules in the interstellar medium as well as in the outflow of carbon stars.


References

  1. Interstellar Processes, ed. D. J. Hollenbach and H. A. Thronson, Reidel, Dordrecht, 1987 Search PubMed.
  2. H. Scheffler and H. Elsässer, Physics of the Galaxy and Interstellar Matter, Springer, Berlin, 1988 Search PubMed.
  3. J. M. Greenberg, Astron. Astrophys., 1971, 12, 240 Search PubMed; A. G. G. M. Tielens and L. J. Allamandola, in ref. 1, p. 397.
  4. D. C. B. Whittet, in Dust and Chemistry in Astronomy, ed. T. J. Millar and D. A. Williams, Institute of Physics, Bristol, 1993, p. 1 Search PubMed; B. Schmitt, in Molecules and Grains in Space, ed. I. Nenner, AIP Press, New York, 1994, p. 735 Search PubMed; W. A. Schutte et al., Astron. Astrophys., 1996, 309, 633 Search PubMed; A. G. G. M. Tielens, L. J. Allamandola and S. A. Sandford, in Solid-State Astrophysics, ed. E. Bussoletti et al., North-Holland, Amsterdam, 1991, p. 29 Search PubMed; J. E. Chiar, A. J. Adamson, T. H. Kerr and D. C. B. Whittet, Astrophys. J., 1995, 426, 240 Search PubMed; R. J. A. Grim and J. M. Greenberg, Astrophys. J. Lett., 1987, 321, 91 Search PubMed; J. H. Lacy, F. Baas, L. J. Allamandola, S. E. Persson, P. J. McGregor, C. J. Lonsdale, T. R. Geballe and C. E. P. van de Bult, Astrophys. J., 1984, 276, 543 Search PubMed; S. C. Tegler, D. A. Weintraub, T. W. Rettig, Y. J. Pendleton, D. C. B. Whittet and C. A. Kulesa, Astrophys. J., 1995, 439, 279; M. E. Palumbo, A. G. G. M. Tielens and A. T. Tokunaga, Astrophys. J., 1995, 449, 674 CrossRef.
  5. L. B. d'Hendecourt and L. J. Allamandola, Astron. Astrophys. Suppl., 1986, 64, 453 Search PubMed; L. J. Allamandola, S. A. Sandford and G. J. Valero, Icarus, 1988, 76, 225 CrossRef CAS; R. J. A. Grim, J. M. Greenberg, M. S. de Groot, F. Baas, W. A. Schutte and B. Schmitt, Astron. Astrophys. Suppl., 1989, 78, 191 Search PubMed; O. M. Shalabiea and J. M. Greenberg, Astron. Astrophys., 1994, 290, 266 Search PubMed.
  6. R. E. Johnson, Energetic Charged Particle Interactions with Atmospheres and Surfaces, Springer, Berlin, 1990 Search PubMed; L. J. Lanzerotti and R. E. Johnson, in Ion Beam Modifications of Insulators, ed. P. G. W. Mazzoldi and E. Arnold, Elsevier, Amsterdam, 1987, p. 631 Search PubMed.
  7. R. E. Johnson, L. J. Lanzerotti and W. L. Brown, Adv. Space Res., 1984, 4, 41 CrossRef CAS; J. Geiss et al., in COSPAR Colloquia Series, ed. E. Marsch and R. Schwenn, Pergamon, New York, 1992, vol. 3, p. 20, and references therein Search PubMed.
  8. K. Roessler, in Solid-State Astrophysics, ed. E. Bussoletti and G. Strazzulla, North-Holland, Amsterdam, 1991, p. 454 Search PubMed.
  9. G. Stöcklin, Chemie heiβer Atome, VCH, Weinheim, 1991 Search PubMed.
  10. R. I. Kaiser and K. Roessler, Astrophys. J., 1997, 475, 144 CrossRef CAS; R. I. Kaiser, G. Eich, A. Gabrysch and K. Roessler, Astrophys. J., 1997, 484, 487 CrossRef CAS; R. I. Kaiser and K. Roessler, Astrophys. J., 1997, submitted Search PubMed.
  11. M. Heyl, Report Jül-2409, 1990.
  12. W. A. Schutte and J. M. Greenberg, Astron. Astrophys., 1991, 244, 190 Search PubMed and references therein R. I. Kaiser, G. Eich, A. Gabrysch and K. Roessler, Astrophys. J., 1997, 484, 487 Search PubMed.
  13. E. L. O. Bakes, The Astrochemical Evolution of the Interstellar Medium, Twin Press, Vledder, 1997 Search PubMed.
  14. Z. K. Alksne, A. K. Alksnis and U. K. Dzervitis, Properties of Galactic Carbon Stars, Orbit, Malabar, 1991 Search PubMed.
  15. E. Herbst and W. Klemperer, Astrophys. J., 1973, 185, 505 CrossRef CAS; E. Herbst, N. G. Adams and D. Smith, Astrophys. J., 1984, 285, 618 CrossRef CAS; G. Winnewisser and E. Herbst, Topic Curr. Chem., 1987, 121 Search PubMed.
  16. T. J. Millar and E. Herbst, Astron. Astrophys., 1994, 288, 561 Search PubMed; I. Cherchneff and A. E. Glassgold, Astrophys. J. Lett., 1993, 419, 41 CrossRef; E. Herbst, H. H. Lee, D. A. Rowe and T. J. Millar, Mon. Not. R. Astron. Soc., 1994, 268, 335 CAS.
  17. D. Husain, J. Chem. Soc., Faraday Trans., 1993, 89, 2164 Search PubMed; D. C. Clary, N. Haider, D. Husain and M. Kabir, Astrophys. J., 1994, 422, 416 CrossRef CAS.
  18. R. D. Levine and R. B. Bernstein, Molecular Reaction Dynamics and Chemical Reactivity, Oxford University Press, Oxford, 1987 Search PubMed.
  19. I. R. Sims et al., J. Chem. Phys., 1994, 100, 4229 CrossRef CAS; I. R. Sims et al., J. Chem. Phys., 1992, 97, 8798 CrossRef CAS; I. R. Sims et al., Chem. Phys. Lett., 1993, 211, 461 CrossRef CAS; I. R. Sims et al., J. Chem. Soc., Faraday Trans., 1994, 90, 1473 RSC.
  20. Y. T. Lee, Science, 1987, 236, 793 CrossRef CAS.
  21. C. Ochsenfeld, R. I. Kaiser, A. G. Suits, Y. T. Lee and M. Head-Gordon, J. Chem. Phys., 1997, 106, 4141 CrossRef CAS.
  22. R. I. Kaiser, C. Ochsenfeld, M. Head-Gordon, Y. T. Lee and A. G. Suits, Science, 1996, 274, 1508 CrossRef CAS.
  23. R. I. Kaiser, Y. T. Lee and A. G. Suits, J. Chem. Phys., 1996, 105, 8705 CrossRef CAS.
  24. R. I. Kaiser, D. Stranges, Y. T. Lee and A. G. Suits, J. Chem. Phys., 1996, 105, 8721 CrossRef CAS.
  25. R. I. Kaiser, D. Stranges, H. M. Bevsek, Y. T. Lee and A. G. Suits, J. Chem. Phys., 1997, 106, 4945 CrossRef CAS.
  26. R. I. Kaiser, W. Sun, A. G. Suits and Y. T. Lee, J. Chem. Phys., 1997, 107, 8713 CrossRef CAS.
  27. J. Keene, K. Young, T. G. Phillips and T. H. Büttgenbach, Astrophys. J. Lett., 1993, 415, 131 CrossRef.
  28. R. I. Kaiser, C. Ochsenfeld, M. Head-Gordon, Y. T. Lee and A. G. Suits, Science, 1996, 274, 1508 CrossRef CAS.
  29. Y. T. Lee, J. D. McDonald, P. R. LeBreton and D. R. Herschbach, Rev. Sci. Instrum., 1969, 40, 1402 CrossRef CAS.
  30. R. I. Kaiser and A. G. Suits, Rev. Sci. Instrum., 1995, 66, 5405 CrossRef CAS.
  31. D. Proch and T. Trickl, Rev. Sci. Instrum., 1989, 60, 713 CrossRef CAS.
  32. G. O. Brink, Rev. Sci. Instrum., 1966, 37, 857 CAS.
  33. N. R. Daly, Rev. Sci. Instrum., 1960, 31, 264 CAS.
  34. M. S. Weiss, PhD Thesis, 1986, University of California, Berkeley.
  35. M. Vernon, PhD Thesis, 1981, University of California, Berkeley.
  36. R. I. Kaiser, C. Ochsenfeld, M. Head-Gordon and Y. T. Lee, Science, submitted Search PubMed.
  37. W. B. Miller, S. A. Safron and D. R. Herschbach, Discuss. Faraday Soc., 1967, 44, 108 291 RSC.
  38. R. I. Kaiser, A. Mebel and Y. T. Lee, J. Chem. Phys., to be submitted Search PubMed.
  39. The zero-point corrections have been calculated for 1-C3D, C2HD at the CCSD(T)(coupled cluster singles and doubles with a perturbative treatment of triple excitations) approximation using a TZP (triple zeta polarization) basis set. For c-C3D the EOMIP-CCSD/TZP (equation of motion CCSD for ionized states) approach was used (R. J. Bartlett and J. F. Stanton, in Reviews of Computational Chemistry, ed. K. B. Lipkowitz and D. B. Boyd, VCH, New York, 1990, p. 65 Search PubMed.
  40. P. Thaddeus et al., Astrophys. J. Lett., 1997, 176, 73 CrossRef.
  41. Y. C. Minh, L. M. Ziurys, W. M. Irvine and D. McGonagle, Astrophys. J., 1991, 366, 192 CrossRef CAS.
  42. E. Herbst, personal communication, 1997.
  43. H. Habara, S. Yamamoto, C. Ochsenfeld, M. Head-Gordon, R. I. Kaiser and Y. T. Lee, J. Chem. Phys., to be submitted Search PubMed.
  44. E. C. Sutton, R. Peng, W. C. Danchi, P. A. Jaminet, G. Sandell and A. P. G. Russel, Astrophys. J. Suppl., 1995, 97, 455 CrossRef CAS; F. Combes, G. Wlodarczak, P. Encrenaz and C. Laurent, Astron. Astrophys., 1992, 253, L29 Search PubMed.
  45. T. J. Millar, P. R. A. Farquhar and K. Willacy, Astron. Astrophys. Suppl., 1997, 121, 139 Search PubMed.
  46. P. Thaddeus, J. M. Vritilek and C. A. Gottlieb, Astrophys. J. Lett., 1985, 299, 63 CrossRef; H. E. Matthews and W. M. Irvine, Astrophys. J. Lett., 1985, 298, 61 CrossRef.
  47. S. Green, Astrophys. J., 1980, 240, 962 CrossRef CAS; B. E. Turner, Astrophys. J. Lett., 1989, 347, L39 CrossRef CAS; P. Thaddeus, J. M. Vrtilek and C. A. Gottlieb, Astrophys. J. Lett., 1985, 299, 63 CrossRef; T. B. Kuiper, J. B. Whiteoak, R. S. Peng, W. L. Peters III and J. E. Reynolds, Astrophys. J. Lett., 1993, 416, 33 CrossRef.
  48. B. E. Turner, L. J. Rickard, L. P. Xu, 1989, 344, 292.
  49. J. Cernicharo et al., Astrophys. J. Lett., 1991, 368, 39 CrossRef.
  50. S. C. Madden, in Chemistry in Space, ed. J. M. Greenberg and V. Pirronello, Kluwer, Dordrecht, 1991, p. 437 and references therein Search PubMed.
  51. S. Yamamoto and S. Saito, Astrophys. J. Lett., 1990, 363, 13 CrossRef.
  52. C. Ochsenfeld, R. I. Kaiser, A. G. Suits, Y. T. Lee and M. Head-Gordon, J. Chem. Phys., 1997, 106, 4141 CrossRef CAS.
  53. A. Mebel, personal communication, 1997.
Click here to see how this site uses Cookies. View our privacy policy here.