Non-local thermodynamic equilibrium in N2O, CH4, and HNO3 in the middle atmosphere

Details Non-local thermodynamic equilibrium in N2O, CH4, and HNO3 in the middle atmosphere Non-local thermodynamic equilibrium in N2O, CH4, and HNO3 in the middle atmosphere

Nov 1997

adsabs.harvard.edu/cgi-bin/nph-data_query?bibcode=1997jastp..59.2167s&link_type=abstract

Journal of Atmospheric and Terrestrial Physics, v. 59, p. 2167-2176.

Physics

7

Scientific paper

This paper presents for the first time theoretical estimates of the non-local thermodynamic equilibrium (NLTE) populations for vibrational states of the N2O and CH4 molecules in the stratosphere and mesosphere. For N2O the nighttime heights of the transition to NLTE decrease with vibrational energy from about 70 km for the (01 10) state to about 55 km for the states excited in the ν3 mode. For daytime the vibrational temperatures of the (0001) state and of higher N2O states far exceed those for nightime. For the N2O (0201, 0221, 1001) states the daytime NLTE layer extends throughout the entire stratosphere. For the first excited states of the CH4 ν2 and ν4 modes the transition to NLTE occurs near 60 km. The vibration-vibration (V-V) energy exchange with N2 and O2 is important in the mesosphere for populating the N2O and CH4 states, respectively. Using the HNO3 molecule as an example, we propose a simple way of estimating roughly the NLTE population of vibrational states of polyatomic molecules when data on the rate constants of vibration-translation (V-T) and V-V energy transfers are lacking. For the HNO3 states not higher than the ν2-state a speculative estimate yields about 50 km as the lower limit for the heights of the transition to NLTE.

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