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Recombination of ozone via the chaperon mechanism
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Image of FIG. 1.
FIG. 1.

(a) Distribution of the rotational angular momentum in the vdW complex for 300 K and several delay times after the preparation of the vdW molecule. (b) Distribution of the total angular momentum of the vdW complex for 300 K and several delay times. In both figures the normalization is such that the area of the distributions is proportional to the number of molecules at a particular delay time.

Image of FIG. 2.
FIG. 2.

Internal energy distributions of the complexes formed in reactions (2c) and (2d) for several temperatures. They are determined at the end of the collisions when Ar has left the complex. Both the complexes in the main wells and in the vdW wells are taken into account.

Image of FIG. 3.
FIG. 3.

Energy and initial-state dependent cross sections for reaction (2c). is the collision energy and is the initial rotational state of . The upper (lower) panel shows the results for definition 1 (2) for the formation of a stable ozone molecule. In these calculations the ArO vdW molecule has no initial internal energy.

Image of FIG. 4.
FIG. 4.

(a) Rate coefficients for the exchange reactions (16a) and (16b) as functions of temperature. For comparison, also the rate coefficient for the exchange reaction is shown. The measured rate for the latter reaction is taken from Ref. 32; because the temperature dependence for the reaction with three isotopes has not been measured, the curve shown is the average of the reaction rates for and as given in Ref. 32. The experiment covers the range from 230 to 350 K. (b) Rate coefficients and for recombination reactions (2c) and (2d), respectively, as functions of temperature. The solid (dashed) lines indicate the results for definition 1 (2) for the formation of a stable ozone molecule. The symbols indicate the temperatures at which calculations have been performed.

Image of FIG. 5.
FIG. 5.

Rate coefficients and for reactions (2c) and (2d), respectively, as functions of the stabilization frequency (in ) in Eq. (9).

Image of FIG. 6.
FIG. 6.

Third-order rate coefficient for definitions 1 (thick solid line) and 2 (thin solid line). Comparison with the estimation of the chaperon rate coefficient of Luther et al. (Ref. 28) (dashed line) and the experimental recombination rate coefficients (• • •). The experimental data are the same as in Ref. 28.

Image of FIG. 7.
FIG. 7.

Third-order rate coefficient for different stabilization frequencies (in ). Comparison with the experimental rate coefficients (• • •).


Generic image for table
Table I.

Relative recombination rate coefficients for two isotope combinations and 300 K.


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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Recombination of ozone via the chaperon mechanism