The H2O-O2 water vapour complex in the Earth's atmosphere

被引:22
作者
Kasai, Y. [1 ]
Dupuy, E. [1 ]
Saito, R. [1 ]
Hashimoto, K. [2 ]
Sabu, A. [2 ]
Kondo, S. [2 ]
Sumiyoshi, Y. [3 ]
Endo, Y. [3 ]
机构
[1] Natl Inst Informat & Commun Technol, Tokyo 1848795, Japan
[2] Tokyo Metropolitan Univ, Dept Chem, Tokyo 1920397, Japan
[3] Univ Tokyo, Dept Basic Sci, Grad Sch Arts & Sci, Meguro Ku, Tokyo 1538902, Japan
关键词
POTENTIAL-ENERGY SURFACE; EQUILIBRIUM-CONSTANT; SPECTROSCOPY; ABSORPTION; VIBRATIONS; O-2-H2O;
D O I
10.5194/acp-11-8607-2011
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Until recently, abundance estimates for bound molecular complexes have been affected by uncertainties of a factor 10-100. This is due to the difficulty of accurately obtaining the equilibrium constant, either from laboratory experiments or by statistical thermodynamic calculations. In this paper, we firstly present laboratory experiments that we performed in order to determine the molecular structure of H2O-O-2. We also derive global abundance estimates for H2O-O-2 in the Earth's atmosphere. The equilibrium constant K-p evaluated using the "anharmonic oscillator approach" (AHOA) (Sabu et al., 2005) was employed: the AHOA explains well the structure of the complex obtained by the present experiment. The K-p calculated by this method shows a realistic temperature dependence. We used this K-p to derive global abundance estimates for H2O-O-2 in the Earth's atmosphere. The distribution of H2O-O-2 follows that of water vapour in the troposphere and seems inversely proportional to temperature in the lower stratosphere. Preliminary estimates at the surface show amount of H2O-O-2 is comparable to CO or N2O, ranking water vapour complexes among the ten most abundant species in the boundary layer.
引用
收藏
页码:8607 / 8612
页数:6
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