FTIR-spectroscopy of molecular clusters in pulsed supersonic slit-jet expansions

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Thomas Häber, Ulrich Schmitt and Martin A. Suhm


Abstract

A new approach to the Fourier transform infrared (FTIR) absorption spectroscopy of molecular clusters in pulsed supersonic jets is developed to the point where it is competitive with high-sensitivity laser absorption techniques for intermediate and large molecular systems. A combination of rapid spectral acquisition and of a buffered jet chamber enables the use of intense gas pulses which cover complete interferometer scans. Applications to (N2O)n, (CH3OH)n and (HCl)n demonstrate the capabilities of this technique. Investigations of the association of bulky alcohols and of clusters within clusters illustrate some ongoing research.


References

  1. A. J. Stone, The Theory of Intermolecular Forces, Clarendon Press, Oxford, 1996 Search PubMed.
  2. L. S. Bartell, Chem. Rev., 1986, 86, 492.
  3. U. Buck, J. Phys. Chem., 1994, 98, 5190 CrossRef CAS.
  4. D. J. Nesbitt, J. Chem. Rev., 1988, 88, 843 Search PubMed.
  5. K. v. Puttkamer and M. Quack, Chem. Phys., 1989, 139, 31 CrossRef.
  6. A. Bizzarri, S. Stolte, J. Reuss, J. G. C. M. van Duijneveldt-van de Rijdt and F. B. van Duijneveldt, Chem. Phys., 1990, 143, 423 CrossRef CAS.
  7. R. J. Bemish, M. Wu and R. E. Miller, Faraday Discuss., 1994, 97, 57 RSC.
  8. M. A. Suhm and D. J. Nesbitt, Chem. Soc. Rev., 1995, 24, 45 RSC.
  9. D. T. Anderson, S. Davis and D. J. Nesbitt, J. Chem. Phys., 1997, 107, 1115 CrossRef CAS.
  10. M. A. Suhm, Ber. Bunsen-Ges. Phys. Chem., 1995, 99, 1159.
  11. K. Kleinermanns, M. Gerhards and M. Schmitt, Ber. Bunsen-Ges. Phys. Chem., 1997, 101, 1785 CAS.
  12. U. Buck, Vibrational spectroscopy of small size-selected clusters, in Molecular Clusters, ed. J. M. Bowman and Z. Bačić, Advances in Molecular Vibrations and Collision Dynamics, JAI Press, London, 1998, \]vol. 3, pp. 127–161 Search PubMed.
  13. P. Rein. ten. Wolde and D. Frenkel, Phys. Chem. Chem. Phys., 1999, 1, 2191 RSC.
  14. M. Quack, U. Schmitt and M. A. Suhm, Chem. Phys. Lett., 1997, 269, 29 CrossRef CAS.
  15. M. Quack, Annu. Rev. Phys. Chem., 1990, 41, 839 CrossRef CAS.
  16. R. A. Provencal, J. B. Paul, K. Roth, C. Chapo, R. N. Casaes, R. J. Saykally, G. S. Tschumper and H. F. Schaefer III, J. Chem. Phys., 1999, 110, 4258 CrossRef CAS.
  17. R. Laenen and C. Rauscher, J. Chem. Phys., 1997, 106, 8974 CrossRef CAS.
  18. J. J. Scherer, J. B. Paul, A. O'Keefe and R. J. Saykally, Chem. Rev., 1997, 97, 25 CrossRef CAS.
  19. J. B. Paul, C. P. Collier, R. J. Saykally, J. J. Scherer and A. O'Keefe, J. Phys. Chem. A, 1997, 101, 5211 CrossRef CAS.
  20. A. Campargue, L. Biennier, A. Kachanov, R. Jost, B. Bussery-Honvault, V. Veyret, S. Churassy and R. Bacis, Chem. Phys. Lett., 1998, 288, 734 CrossRef CAS.
  21. P. Asselin, B. Dupuis, J. P. Perchard and P. Soulard, Chem. Phys. Lett., 1997, 268, 265 CrossRef CAS.
  22. A. Amrein, M. Quack and U. Schmitt, J. Phys. Chem., 1988, 92, 5455 CrossRef CAS.
  23. R. Campargue, J. Phys. Chem., 1984, 88, 4466 CrossRef CAS.
  24. J. A. Barnes and T. E. Gough, Chem. Phys. Lett., 1986, 130, 297 CrossRef CAS.
  25. J. A. Barnes and T. E. Gough, J. Chem. Phys., 1987, 86, 6012 CrossRef CAS.
  26. C. L. Hartz, B. A. Wofford, R. F. Meads, R. R. Lucchese and J. W. Bevan, Rev. Sci. Instrum., 1995, 66, 4375 CrossRef CAS.
  27. R. Georges, G. Durry, M. Bach, R. Peétrisse, R. Jost and M. Herman, Chem. Phys. Lett., 1995, 246, 601 CrossRef CAS.
  28. S. Tanimura, Y. Okada and K. Takeuchi, J. Chem. Phys., 1997, 107, 7096 CrossRef CAS.
  29. C. M. Lovejoy and D. J. Nesbitt, Rev. Sci. Instrum., 1987, 58, 807 CrossRef CAS.
  30. K. Liu, R. S. Fellers, M. R. Viant, R. P. McLaughlin, M. G. Brown and R. J. Saykally, Rev. Sci. Instrum., 1996, 67, 410 CrossRef CAS.
  31. D. Luckhaus, M. Quack, U. Schmitt and M. A. Suhm, Ber. Bunsen-Ges. Phys. Chem., 1995, 99, 457 CAS.
  32. We suggest the french (culinary) pronunciation of ragout, bearing in mind the high number density of large clusters dispersed in a rare gas fluid, which can be generated in such an experiment.
  33. M. Gauthier, J. Chem. Phys., 1988, 88, 5439 CrossRef CAS.
  34. C. L. Lugez, F. J. Lovas, J. T. Hougen and N. Ohashi, J. Mol. Spectrosc., 1999, 194, 95 CrossRef CAS.
  35. Photographs of the setup can be found on our web-site http://www-suhm.uni-pc.gwdg.de.
  36. D. Zimmermann, T. Häber and M. A. Suhm, in preparation.
  37. E. Alexopoulos, N. Borho, T. Häber, D. Zimmermann and M. A. Suhm, in preparation.
  38. R. E. Miller, R. O. Watts and A. Ding, Chem. Phys., 1984, 83, 155 CrossRef CAS.
  39. Z. S. Huang and R. E. Miller, J. Chem. Phys., 1988, 89, 5408 CrossRef CAS.
  40. Y. Ohshima, Y. Matsumoto, M. Takami and K. Kuchitsu, Chem. Phys. Lett., 1988, 152, 294 CrossRef CAS.
  41. T. E. Gough, R. E. Miller and G. Scoles, J. Chem. Phys., 1978, 69, 1588 CrossRef CAS.
  42. R. E. Miller and L. Pedersen, J. Chem. Phys., 1998, 108, 436 CrossRef CAS.
  43. R. E. Miller and L. Pedersen, Chem. Phys. Lett., 1997, 275, 307 CrossRef CAS.
  44. D. R. Miller, Free Jet Sources, in Atomic and Molecular Beam Methods, ed. G. Scoles, Oxford University Press, Oxford, 1988 Search PubMed.
  45. A. E. Beylich, Z. Flugwiss. Weltraumforsch., 1979, 3, 48 Search PubMed.
  46. D. J. Creasey, D. E. Heard, M. J. Pilling, B. J. Whitaker, M. Berzins and R. Fairlie, Appl. Phys. B, 1997, 65, 375 CrossRef.
  47. I. Suzuki, J. Mol. Spectrosc., 1969, 32, 54 CrossRef CAS.
  48. J. E. Cahill and N. Ali, Chem. Phys. Lett., 1977, 45, 504 CrossRef CAS.
  49. D. A. Dows, J. Chem. Phys., 1957, 26, 745 CrossRef CAS.
  50. A. Anderson and T. S. Sun, Chem. Phys. Lett., 1971, 8, 537 CrossRef CAS.
  51. R. Disselkamp and G. E. Ewing, J. Chem. Phys., 1993, 99, 2439 CrossRef CAS.
  52. W. G. Lawrence and V. A. Apkarian, J. Chem. Phys., 1992, 97, 2224 CrossRef CAS.
  53. F. Huisken, M. Kaloudis, M. Koch and O. Werhahn, J. Chem. Phys., 1996, 105, 8965 CrossRef.
  54. S. Coussan, A. Loutellier, J. P. Perchard, S. Racine, A. Peremans, A. Tadjeddine and W. Q. Zheng, J. Chem. Phys., 1998, 107, 6526 CrossRef CAS.
  55. M. Behrens, R. Fröchtenicht, M. Hartmann, J.-G. Siebers, U. Buck and F. C. Hagemeister, J. Chem. Phys., 1999, 111, 2436 CrossRef CAS.
  56. G. S. Tschumper, J. M. Gonzales and H. F. Schaefer III, J. Chem. Phys., 1999, 111, 3027 CrossRef CAS.
  57. M. Quack and M. A. Suhm, Spectroscopy and Quantum Dynamics of Hydrogen Fluoride Clusters, in Molecular Clusters ed. J. M. Bowman and Z. Bačić, Advances in Molecular Vibrations and Collision Dynamics, JAI Press, London, 1998, vol. 3, pp. 205–248 Search PubMed.
  58. H. Schaal, T. Häber and M. A. Suhm, J. Phys. Chem. A, 1999, 103 Search PubMed in the press.
  59. U. Buck and H. Meyer, Phys. Rev. Lett., 1984, 52, 109 CrossRef CAS.
  60. U. Buck and I. Ettischer, J. Chem. Phys., 1998, 108, 33 CrossRef CAS.
  61. O. V. Boyarkin, T. R. Rizzo and D. S. Perry, J. Chem. Phys., 1999, 110, 11346 CrossRef CAS.
  62. C. J. Gruenloh, G. M. Florio, J. R. Carney, F. C. Hagemeister and T. S. Zwier, J. Phys. Chem. A, 1999, 103, 496 CrossRef CAS.
  63. M. Quack and M. Willeke, J. Chem. Phys., 1999, 110, 11958 CrossRef CAS.
  64. V. Hänninen, M. Horn and L. Halonen, J. Chem. Phys., 1999, 111, 3018 CrossRef CAS.
  65. M. Falk and E. Whalley, J. Chem. Phys., 1961, 34, 1554 CAS.
  66. L. Gonzáles, O. Mo and M. Yáñez, J. Chem. Phys., 1999, 111, 3855 CrossRef.
  67. C. Perchard and J. P. Perchard, J. Raman Spectrosc., 1975, 3, 277 CAS.
  68. S. Sarkar and R. N. Joarder, J. Chem. Phys., 1994, 100, 5118 CrossRef CAS.
  69. W. A. P. Luck and M. Fritzsche, Z. Phys. Chem., 1995, 191, 71 CAS.
  70. D. T. Bowron, J. L. Finney and A. K. Soper, Mol. Phys., 1998, 93, 531 CrossRef CAS.
  71. R. Laenen, K. Simeonidis and R. J. Ludwig, J. Chem. Phys., 1999, 111, 5897 CrossRef CAS.
  72. J. H. van der Maas and E. T. G. Lutz, Spectrochim. Acta, 1974, 30A, 2005 CrossRef.
  73. F. A. Smith and E. C. Creitz, J. Res. Natl. Bur. Standards, 1951, 46, 145 Search PubMed.
  74. E. D. Becker, E. E. Tucker and C. N. R. Rao, J. Chem. Soc., Faraday Trans. 2, 1977, 73, 438 RSC.
  75. M. Kunst, D. van Duijn and P. Bordewijk, Ber. Bunsen-Ges. Phys. Chem., 1978, 82, 1073 Search PubMed.
  76. R. Laenen and K. Simeonidis, Chem. Phys. Lett., 1998, 290, 94 CrossRef CAS.
  77. A. Furlan, S. Wülfert and S. Leutwyler, Chem. Phys. Lett., 1988, 153, 291 CrossRef CAS.
  78. M. D. Schuder, C. M. Lovejoy, R. Lascola and D. J. Nesbitt, J. Chem. Phys., 1993, 99, 4346 CrossRef CAS.
  79. A. J. Barnes, H. E. Hallam and G. F. Scrimshaw, Trans. Faraday Soc., 1969, 65, 3150 RSC.
  80. B. J. v. d. Veken and F. R. DeMunck, J. Chem. Phys., 1992, 97, 3060 CrossRef CAS.
  81. A. S. Pine and B. J. Howard, J. Chem. Phys., 1986, 84, 590 CrossRef CAS.
  82. N. Moazzen-Ahmadi, A. R. W. McKellar and J. W. C. Johns, J. Mol. Spectrosc., 1989, 138, 282 CrossRef CAS.
  83. G. Chałasiński, S. M. Cybulski, M. M. Szczȩśniak and S. Scheiner, J. Chem. Phys., 1989, 91, 7048 CrossRef CAS.
  84. A. Karpfen, P. R. Bunker and P. Jensen, Chem. Phys., 1991, 149, 299 CrossRef CAS.
  85. M. J. Elrod and R. J. Saykally, J. Chem. Phys., 1995, 103, 921 CrossRef CAS.
  86. Y. Qiu and Z. Bačić, J. Chem. Phys., 1997, 106, 2158 CrossRef CAS.
  87. Z. Latajka and S. Scheiner, Chem. Phys., 1997, 216, 37 CrossRef CAS.
  88. M. J. Frisch, et al.“GAUSSIAN98, Revision A.3”, Gaussian Inc., Pittsburgh PA, 1998.
  89. C. Votava, R. Ahlrichs and A. Geiger, J. Chem. Phys., 1983, 78, 6841 CrossRef CAS.
  90. M. Quack and M. A. Suhm, Potential Energy Hypersurfaces for Hydrogen Bonded Clusters (HF)n, in Conceptual Perspectives in Quantum Chemistry, ed. J.-L. Calais and E. S. Kryachko, Conceptual Trends in Quantum Chemistry, Kluwer, Dordrecht, 1997, vol. 3, pp. 415–463 Search PubMed.
  91. F. Huisken and M. Staemmler, J. Chem. Phys., 1993, 98, 7680 CrossRef CAS.
  92. M. Lewerenz, J. Chem. Phys., 1996, 104, 1028 CrossRef CAS.
  93. B. Schmidt and P. Jungwirth, Chem. Phys. Lett., 1996, 259, 62 CrossRef CAS.
  94. A. V. Nemukhin, B. L. Grigorenko and A. V. Savin, Chem. Phys. Lett., 1996, 250, 226 CrossRef CAS.
  95. D. Green, S. Hammond, J. Keske and B. H. Pate, J. Chem. Phys., 1999, 110, 1979 CrossRef CAS.
  96. M. Rasanen, J. Murto and V. E. Bondybey, J. Phys. Chem., 1985, 89, 3967 CrossRef CAS.
  97. J. Timmler and P. Roth, Part. Part. Syst. Charact., 1991, 8, 79 CAS.
  98. S. Bauerecker, F. Taucher, C. Weitkamp and H. K. Cammenga, Multireflection flow-cooling cell for IR spectroscopy of supercooled gases, in Proceedings of the SPIE: Application of Tunable Diode and Other Infrared Sources for Atmospheric Studies and Industrial Process Monitoring, ed. A. Fried, 1996, vol. 2834, pp. 257–261 Search PubMed.
  99. M. Halupka and W. Sander, Spectrochim. Acta, 1998, 54, 495 CrossRef.
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