Freezing of HNO3/H2SO4/H2O solutions at stratospheric temperatures: Nucleation statistics and experiments

Journal of Physical Chemistry A

Volumn 101, Issue 6, 1997, Pages 1117-1133

  Koop, Thomas ^a   Luo, Beiping ^a   Biermann, Uta M ^a   Crutzen, Paul J ^a   Peter, Thomas ^a  

^a MAX PLANCK INSTITUTE FOR CHEMISTRY   (Germany)

Author keywords

[No Author keywords available]

Indexed keywords

ATMOSPHERIC TEMPERATURE; CRYSTAL GROWTH; HYDRATES; HYDROGEN INORGANIC COMPOUNDS; NUCLEATION; PHASE EQUILIBRIA; RANDOM PROCESSES; STATISTICAL METHODS; THERMODYNAMIC PROPERTIES;

FREEZING PROBABILITY; POISSON STATISTICS; STRATOSPHERIC TEMPERATURES; THERMODYNAMIC EQUILIBRIUM;

FREEZING;

EID: 0031555742     PISSN: 10895639     EISSN: None     Source Type: Journal    
DOI: 10.1021/jp9626531     Document Type: Article

References (69)

1. Carslaw, K. S.; Luo, B. P.; Clegg, S. L.; Peter, Th.; Brimblecombe, P; Crutzen, P. J. Geophys. Res. Lett. 1994, 21, 2479-2482.
2. Tabazadeh, A.; Turco, R. P.; Drdla, K.; Jacobson, M. Z.; Toon, O. B. Geophys. Res. Lett. 1994, 21, 1619-1622.
3. Drdla, K.; Tabazadeh, A.; Turco, R. P.; Jacobson, M. Z.; Dye, J. E.; Twohy, C.; Baumgardner, D.; Kelly, K. K.; Chan, R. P.; Loewenstein, M. Geophys. Res. Lett. 1994, 21, 2473-2478.
4. Toon, O. B.; Browell, E. V.; Kinne, S.; Jordan, J. Geophys. Res. Lett. 1990, 17, 393-396.
5. Beyerle, G.; Luo, B. P.; Neuber, R.; Peter, T.; McDermid, I. S., submitted to J. Geophys. Res.
6. Dye, J. E.; Baumgardner, D.; Gandrud, B. W.; Kawa, S. R.; Kelly, K. K.; Loewenstein, M.; Ferry, G. V.; Chan, K. R.; Gary, B. L. J. Geophys. Res. 1992, 97, 8015-8034.
7. Dye, J. E., Baumgardner, D.; Gandrud, B. W.; Drdla, K.; Barr, K.; Fahey, D. W.; Delnegro, L. A.; Tabazadeh, A.; Jonsson, H. H.; Wilson, J. C.; Loewenstein, M.; Podolske, J.; Chan, K. R. Geophys. Res. Lett. 1996, 23, 1913-1916.
8. Poole, L. R.; McCormick, M. P. J. Geophys. Res. 1988, 93, 8423-8430.
9. Crutzen, P. J.; Arnold, F. Nature 1986, 324, 651-655.
10. Toon, O. B.; Hamill, P.; Turco, R. P.; Pinto, J. Geophys. Res. Lett. 1986, 13, 1284-1287.
11. Hanson, D.; Mauersberger, K. Geophys. Res. Lett. 1988, 15, 855-858.
12. Browell, E. V.; Butler, C. F.; Ismail, S.; Robinette, P. A.; Carter, A. F.; Higdon, N. S.; Toon, O. B.; Schoeberl, M. R.; Tuck, A. F. Geophys. Res. Lett. 1990, 17, 385-388.
13. Beyerle, G.; Neuber, R.; Schrems, O.; Wittrock, F.; Knudsen, B. Geophys. Res. Lett. 1994, 21, 57-60.
14. Rosen, J. M.; Kjome, N. T.; Oltmans, S. J. J. Geophys. Res. 1993, 98, 12741-12751.
15. Molina, M. J.; Zhang, R.; Wooldridge, P. J.; McMahon, J. R.; Kim, J. E.; Chang, H. Y.; Beyer, K. D. Science 1993, 261, 1418-1423.
16. Iraci, L. T.; Middlebrook, A. M.; Wilson, M. A.; Tolbert, M. A. Geophys. Res. Lett. 1994, 21, 867-870.
17. Worsnop, D. R.; Fox, L. E.; Zahniser, M. S.; Wofsy, S. C. Science 1993, 259, 71-74.
18. Marti, J.; Mauersberger, K. J. Phys. Chem. 1994, 98, 6897-6899.
19. Fox, L. E., Worsnop, D. R.; Zahniser, M. S.; Wofsy, S. C. Science 1995, 267, 351-355.
20. Tabazadeh, A.; Toon, O. B. J. Geophys. Res. 1996, 101, 9071-9078.
21. Koop, T.; Biermann, U. M.; Raber, W.; Luo, B. P.; Crutzen, P. J.; Peter, Th. Geophys. Res. Lett. 1995, 22, 917-920.
22. Tabazadeh, A.; Toon, O. B.; Hamill, P. Geophys. Res. Lett. 1995, 22, 1725-1728.
23. Meilinger, S. K.; Koop, T.; Luo, B. P.; Huthwelker, T.; Carslaw, K. S.; Krieger, U.; Crutzen, P. J.; Peter, Th. Geophys. Res. Lett. 1995, 22, 3031-3034.
24. Molina M. J. In The Chemistry of the Atmosphere: The Impact of Global Change; Calvert, J. G., Ed.; Blackwell Scientific Publishers: Oxford, U.K., 1994.
25. Ravishankara, A. R; Hanson, D. R. J. Geophys. Res. 1996, 101, 3885-3890.
26. Carslaw, K. S.; Peter, Th. In Polar stratospheric ozone, Proceedings of the 3rd European workshop, Schliersee, Germany, 1995; Pyle, J. A., Harris, N. R. P., Amanatidis, G. T., Eds.; European Commission Publication Office: Luxembourg, 1996.
27. Hanson, D. R.; Ravishankara, A. R.; Solomon, S. J. Geophys. Res. 1994, 99, 3615-3629.
28. Iraci, L. T.; Middlebrook, A. M.; Tolbert, M. A. J. Geophys. Res. 1995, 100, 20969-20977.
29. Ohtake, T. Tellus 1993, 45B, 138-144.
30. Beyer, K. D. Laboratory experiments of chemical reactions on PSC particles. Ph.D. Thesis, Massachusetts Institute of Technology, Cambridge, MA, 1994.
31. Beyer, K. D.; Seago, S. W.; Chang, H. Y.; Molina, M. J. Geophys. Res. Lett. 1994, 216, 871-874.
32. Song, N. Geophys. Res. Lett. 1994, 21, 2709-2712.
33. Anthony, S. E.; Tisdale, R. T.; Disselkamp, R.; Tolbert, M. A.; Wilson, J. C. Geophys. Res. Lett. 1995, 22, 1105-1108.
34. Disselkamp, R. S.; Anthony, S. E.; Prenni, A. J.; Onasch, T. B.; Tolbert, M. A. J. Phys. Chem. 1996, 100, 9127-9137.
35. Bertram, A. K.; Patterson, D. D.; Sloan, J. J. J. Phys. Chem. 1996, 100, 2376-2383.
36. Note that the probability p for a single molecule to become the center of a critical nucleus is proportional to the observation time t for t ≪ mp/ω but saturates (p → 1) for t ≫ mp/ω. The probability for no nucleation obeys the equation d(1 - p)/dt = - (ω/m)(1 - p) with the solution 1 - p = exp(-ωt/m), which resembles the decay law eq 4 for the entire sample.
37. Barlow, T. W.; Haymet, A. D. J. Rev. Sci. Instrum. 1995, 66, 2996-3007.
38. Pruppacher, H. R.; Klett, J. D. Microphysics of Clouds and Precipitation; D. Reidel Publishing Co.: Dordrecht, Holland, 1978.
39. See also: Regener, V. H. Phys. Rev. 1951, 84, 161-162. Brandt, S. Datenanalyse, 3rd ed.; BI-Wissenschaftsverlag: Mannheim, 1992.
40. See also: Regener, V. H. Phys. Rev. 1951, 84, 161-162. Brandt, S. Datenanalyse, 3rd ed.; BI-Wissenschaftsverlag: Mannheim, 1992.
41. Larsen, N.; Knudsen, B. M.; Rosen, J. M.; Kjome, N. T.; Kyro, E. Geophys. Res. Lett. 1996, 23, 1091-1094.
42. Ha, A.; Cohen, I.; Zhao, X.; Lee, M.; Kivelson, D. J. Phys. Chem. 1996, 100, 1-4.
43. A glass point is the temperature at which a liquid turns into a glass upon cooling as evidenced by changes in its thermodynamic properties (i.e. molar volume, enthalpy, entropy, heat capacity, viscosity etc.). Strictly speaking, the glass point depends on the cooling rate applied to the system; however, for our purpose it is sufficient to think of it as being one single temperature which depends only on concentration.
44. Cohen, I.; Ha, A.; Zhao, X.; Lee, M.; Fischer, T.; Strouse, M. J.; Kivelson, D. J. Phys. Chem. 1996, 100, 8518-8526.
45. Johari, G. P.; Hallbrucker, A.; Mayer, E. Science 1996, 273, 90-92.
46. Barton, N., Rowland, B.; Devlin, J. P. J. Phys. Chem. 1993, 97, 5848-5851.
47. Tolbert, M. A.; Koehler, B. G.; Middlebrook, A. M. Spectrochim. Acta 1992, 48A, 1303-1313.
48. Tang, I. N.; Fung, K. H.; Imre, D. G.; Munkelwitz, H. R. Aerosol Sci. Technol. 1995, 23, 443-453.
49. Tang, I. N.; Munkelwitz, H. R. Atmos. Environ. 1993, 27A, 467-473.
50. Luo, B. P.; Carslaw, K. S.; Peter, Th.; Clegg, S. Geophys. Res. Lett. 1995, 22, 247-250.
51. Gable, C. M.; Betz, H. F.; Maron, S. H. J. Am. Chem. Soc. 1950, 72, 1445-1448.
52. Mootz, D.; Merschenz-Quack, A. Z. Naturforsch. 1987, 42b, 1231-1236.
53. Wood, G. R.; Walton, A. G. J. Appl. Phys. 1970, 41, 3027-3036.
54. Middlebrook, A. M.; Iraci, L. T.; McNeill, L. S.; Koehler, B. G.; Wilson, M. A.; Saastad, O. W.; Tolbert, M. A.; Hanson, D. R. J. Geophys. Res. 1993, 98, 20473-20481.
55. Biermann, U. M.; Presper, T.; Koop, T.; Mössinger, J.; Crutzen, P. J.; Peter, Th. Geophys. Res. Lett. 1996, 23, 1693-1696.
56. Kärcher, B.; Peter, Th.; Biermann, U. M.; Schumann, U. J. Atmos. Sci. 1996, 53, 3066-3083.
57. Luo, B. P.; Peter, Th.; Crutzen, P. Geophys. Res. Lett. 1994, 21, 1447-1450.
58. Schäfer, K. In Landolt-Börnstein Serie, II. Band, 5. Teil; Springer Verlag: Heidelberg, 1969.
59. Williams, L. R.; Golden, D. M. Geophys. Res. Lett. 1993, 20, 2227-2230.
60. Williams, L. R.; Long, F. S. J. Phys. Chem. 1995, 99, 3745-3751.
61. 3 shown in Figure 6 is not subject to such a procedure. It does not suffer from unintended seeding because of the high temperature (226 K).
62. 3, respectively.
63. Hanson, D. R. Geophys. Res. Lett. 1992, 19, 2063-2066.
64. The approximation in eq A2 requires |ε| ≪ k and |ε| ≪ m - k. This is satisfied for all relevant values of k and x.
65. Vuillard, G. Bull. Soc. Chim. 1954, 802-807.
66. 2O. Ph.D. Thesis, L'université de Paris, Paris, 1994.
67. Zhang, R., Laboratory investigations of heterogeneous chemistry important to ozone depletion in the stratosphere. Ph.D. Thesis, Massachusetts Institute of Technology, Cambridge, MA, 1993.
68. Küster, F. W.; Kremann, R. Z. Anorg. Chem. 1904, 41, 1-42.
69. Satoh, K.; Kanno, H. Bull. Chem. Soc. Jpn. 1982, 55, 1645-1646.